Dissertations from 2018 to 2021

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Li, Feitao; Tan, Xinu; Flock, Dominik; Qiu, Risheng; Wang, Dong; Schaaf, Peter
Formation of CuO whiskers and facet-controlled oxidation during the oxidation of Au-Cu nanoparticles fabricated by solid-state dewetting. - In: Applied surface science, Bd. 610 (2023), 155547

The fabrication of cupric oxide (CuO) nanowires from Cu particles via thermal oxidation provides a simple and scalable method to produce hierarchical structures. A stress-induced growth mechanism is believed to account for the nanowire formation while a slow oxidation rate is favored to sustain the driving force. Here, CuO whiskers are grown from Au-Cu nanoparticles because the formation of Au-Cu phases decreases the Cu diffusion rate and in turn slows down the oxidation rate. The driving force for the whisker growth is attributed to the compressive stress imposed by the CuO shell on the Au-Cu core, which is induced by the significantdifference in their linear thermal expansion coefficients. The contribution of the compressive stress is proved by the calculation. Moreover, preferred oxidation is observed and it is related to the crystalline structures of different facets existing on the surface of Au-Cu nanoparticles. The more compact the plane, the slower the diffusion rate through the plane, resulting in the formation of thinner CuO on the relevant facet. The results open a cost-effect way to fabricate hybrid nanostructures consisting of Cu-based core-shell nanoparticles attached with CuO whiskers and bring new insights into the oxidation behaviors of Cu on different crystal planes.



https://doi.org/10.1016/j.apsusc.2022.155547
Liang, Zhengchen; Wang, Dong; Ziegler, Mario; Hübner, Uwe; Xie, Peng; Ding, Qi; Zhang, Hong; Wang, Wei
Coupling-induced tunable broadband superradiance in 2D metal-dielectric-metal nanocavity arrays. - In: Laser & photonics reviews, ISSN 1863-8899, Bd. 16 (2022), 11, 2200393, S. 1-8

Subradiance/superradiance, cooperative effects causing suppressed/enhanced radiative decay, are of particular interest in plasmonic systems as they play a very important role in modulating dampings and optical properties of resonant systems. However, subradiance/superradiance are generally limited in narrow spectral range with inaccessible tunability. Realizing broadband subradiant and superradiant plasmon modes with flexible tuning is still challenging. Here, a 2D periodic multilayer metal-dielectric-metal (MDM) nanostructure is rationally designed and fabricated to realize a tunable superradiant mode over a broad visible range. Angle-resolved spectroscopy combined with full quantum calculations reveal a sufficient hybridization of delocalized guided plasmons with localized plasmons and a plasmonic cavity mode, leading to an emissive superradiant hybrid mode over a broadband visible range, which can be readily tuned by controlling the spectral three-mode overlap. Greatly shortened polariton lifetimes down to 4 fs are achieved as direct consequence of the Rabi phases and considerable incoherent coupling strengths between interacting subsystems. Such a control of plasmon damping by cooperative mode interactions paves the way toward efficient manipulation of light emission for applications requiring bright, fast-emitting photon sources.



https://doi.org/10.1002/lpor.202200393
Jaekel, Konrad; Bartsch, Heike; Müller, Jens; Sauni Camposano, Yesenia Haydee; Matthes, Sebastian; Schaaf, Peter
Effect of line structures on the self-propagating reaction of Al/Ni multilayer. - In: IEEE Xplore digital library, ISSN 2473-2001, (2022), S. 379-382

This work investigates the influence of a structured chip surface on the propagation of a self-sustaining reaction that is aimed to be used as heat source for chip assembly. A silicon (100) surface was structured by a combination of thermal oxidation and dry and wet etching to obtain line structures with height lesser than 1 µm. To ensure reaction of 5 µm thick Al/Ni multilayers, 1 µm of SiO2 is used as thermal insulator. Different widths of lines and valleys, with a ratio of 1:1, were processed. Width values were chosen to be 30 µm, 50 µm and 80 µm. Bilayer thickness of 50 nm with a 50/50 at% of Al/Ni were deposited using magnetron sputtering. By using focused ion beam with integrated scanning electron microscope and X-ray diffractometer the samples were analyzed prior to reaction. Velocity and temperature were measured with high-speed camera and high-speed pyrometer. Variations in reaction speed depending on the structure width were recorded and analyzed in perspective of the influence of the additional inclined reaction path. Calculation of the extended reaction paths and their influence on the reaction speed between the structures was performed. The results show that the additional distance has only a low influence on the velocity. Different reasons were identified, but it was not possible to determine the main cause. It was possible to slow down the reaction and keeping the temperature over 350 ˚C for over 500 ms, which provides enough energy to melt solders. The influence of smaller structures can be applied to bonding applications with reactive multilayers.



https://doi.org/10.1109/ESTC55720.2022.9939472
Kurtash, Vladislav; Mathew, Sobin; Thiele, Sebastian; Scheler, Theresa; Reiprich, Johannes; Hähnlein, Bernd; Stauffenberg, Jaqueline; Manske, Eberhard; Narasimha, Shilpashree; Abedin, Saadman; Jacobs, Heiko O.; Pezoldt, Jörg
Hysteresis associated with intrinsic-oxide traps in gate-tunable tetrahedral CVD-MoS2 memristor. - In: IEEE Xplore digital library, ISSN 2473-2001, (2022), S. 527-530

We introduce back gated memristor based on CVD-grown 30-40 nm thick MoS2 channel. The device demonstrates bipolar behaviour and the measurements are consistent with the simulations performed within the intrinsic-oxide traps model. This confirms the theory that the source of hysteresis in thin-film MoS2 memristors is charge trapping on MoS2/SiO2 interface and the grain boundaries. The impact of back gate voltage bias, voltage sweep range and channel area on memristive effect was studied and quantified using hysteresis area. Hysteresis in bipolar memristors can be tuned by back gate voltage, which makes these devices promising for neuromorphic computing.



https://doi.org/10.1109/NANO54668.2022.9928717
Quispe, Roger; Torres, Carlos; Eggert, Lara; Ccama, Gianella A.; Kurniawan, Mario; Hopfeld, Marcus; Zárate Moya, José Luis; Camargo, Magali K.; Rosenkranz, Andreas; Acosta, Julio A.; Bund, Andreas; Schaaf, Peter; Grieseler, Rolf
Tribological and mechanical performance of Ti2AlC and Ti3AlC2 thin films. - In: Advanced engineering materials, ISSN 1527-2648, Bd. 24 (2022), 10, 2200188, S. 1-11

Mn+1AXn (MAX) phases are novel structural and functional materials with a layered crystal structure. Their unique properties such as good machinability, high electrical conductivity, low friction, and corrosion resistance are appealing for many engineering applications. Herein, Ti2AlC and Ti3AlC2 MAX thin films are synthesized by magnetron sputtering and subsequent thermal annealing. A multilayer approach is used to deposit single-element nanolayers of titanium, aluminum, and carbon onto silicon substrates with a double-layer-diffusion barrier of SiO2 and SixNy. Ti2AlC and Ti3AlC2 thin films (thickness ≈500 nm) are formed via rapid thermal annealing and verified by X-Ray diffraction. Nanoindentation tests show hardness values of about 11.6 and 5.3 GPa for Ti2AlC and Ti3AlC2, respectively. The tribological behavior of the Ti2AlC and Ti3AlC2 thin films against AISI 52100 steel balls under dry sliding conditions is studied using ball-on-flat tribometry. The resulting coefficient of friction (CoF) for Ti2AlC and Ti3AlC2 ranges between 0.21-0.42 and 0.64-0.91, respectively. The better tribological behavior observed for Ti2AlC thin films is ascribed to its smaller grain size, reduced surface roughness, and higher hardness.



https://doi.org/10.1002/adem.202200188
Mathew, Sobin; Narasimha, Shilpashree; Reiprich, Johannes; Scheler, Theresa; Hähnlein, Bernd; Thiele, Sebastian; Stauffenberg, Jaqueline; Kurtash, Vladislav; Abedin, Saadman; Manske, Eberhard; Jacobs, Heiko O.; Pezoldt, Jörg
Formation and characterization of three-dimensional tetrahedral MoS2 thin films by chemical vapor deposition. - In: Crystal growth & design, ISSN 1528-7505, Bd. 22 (2022), 9, S. 5229-5238

A method to synthesize the three-dimensional arrangement of bulk tetrahedral MoS2 thin films by solid source chemical vapor deposition of MoO3 and S is presented. The developed synthesizing recipe uses a temperature ramping with a constant N2 gas flow in the deposition process to grow tetrahedral MoS2 thin film layers. The study analyses the time-dependent growth morphologies, and the results are combined and presented in a growth model. A combination of optical, electron, atomic force microscopy, Raman spectroscopy, and X-ray diffraction are used to study the morphological and structural features of the tetrahedral MoS2 thin layers. The grown MoS2 is c-axis oriented 2H-MoS2. Additionally, the synthesized material is further used to fabricate back-gated field-effect transistors (FETs). The fabricated FET devices on the tetrahedral MoS2 show on/off current ratios of 10^6 and mobility up to ∼56 cm^2 V^-1 s^-1 with an estimated carrier concentration of 4 × 10^16 cm-3 for VGS = 0 V.



https://doi.org/10.1021/acs.cgd.2c00333
Dang, Thien Thanh; Schell, Juliana; Boa, Andrea González; Lewin, Daniil; Marschick, Georg; Dubey, Astita; Escobar-Castillo, M.; Noll, Cornelia; Beck, Reinhard; Zyabkin, Dmitry; Glukhov, Konstantin E.; Yap, Ian Chang Jie; Mokhles Gerami, Adeleh; Lupascu, Doru C.
Temperature dependence of the local electromagnetic field at the Fe site in multiferroic bismuth ferrite. - In: Physical review, ISSN 2469-9969, Bd. 106 (2022), 5, S. 054416-1-054416-15

In this paper, we present a study of the temperature-dependent characteristics of electromagnetic fields at the atomic scale in multiferroic bismuth ferrite (BiFeO3 or BFO). The study was performed using time differential perturbed angular correlation (TDPAC) spectroscopy on implanted 111In (111Cd) probes over a wide temperature range. The TDPAC spectra show that substitutional 111In on the Fe3+ site experiences local electric polarization, which is otherwise expected to essentially stem from the Bi3+ lone pair electrons. Moreover, the TDPAC spectra show combined electric and magnetic interactions below the Néel temperature TN. This is consistent with simulated spectra. X-ray diffraction (XRD) was employed to investigate how high-temperature TDPAC measurements influence the macroscopic structure and secondary phases. With the support of ab initio DFT simulations, we can discuss the probe nucleus site assignment and can conclude that the 111In (111Cd) probe substitutes the Fe atom at the B site of the perovskite structure.



https://doi.org/10.1103/PhysRevB.106.054416
Haas, Heinz; Zyabkin, Dmitry; Schell, Juliana; Dang, Thien T.; Yap, Ian C. J.; Michelon, Ilaria; Gaertner, Daniel; Gerami, Adeleh Mokhles; Noll, Cornelia; Beck, Reinhard
Confirming the unusual temperature dependence of the electric-field gradient in Zn. - In: Crystals, ISSN 2073-4352, Bd. 12 (2022), 8, 1064, S. 1-8

The electric-field gradient (EFG) at nuclei in solids is a sensitive probe of the charge distribution. Experimental data, which previously only existed in insulators, have been available for metals with the development of nuclear measuring techniques since about 1970. An early, systematic investigation of the temperature dependence of the EFG in metals, originally based on results for Cd, but then also extended to various other systems, has suggested a proportionality to T3/2. However, later measurements in the structurally and electronically similar material Zn, which demonstrated much more complex behavior, were largely ignored at the time. The present experimental effort has confirmed the reliability of this unexpected behavior, which was previously unexplained.



https://doi.org/10.3390/cryst12081064
Cheng, Pengfei; Wang, Dong; Schaaf, Peter
A review on photothermal conversion of solar energy with nanomaterials and nanostructures: from fundamentals to applications. - In: Advanced sustainable systems, ISSN 2366-7486, Bd. 6 (2022), 9, 2200115, S. 1-19

Solar energy is a green, sustainable, and de facto inexhaustible energy source for mankind. The conversion of solar energy into other forms of energy has attracted extensive research interest due to climate change and the energy crisis. Among all the solar energy conversion technologies, photothermal conversion of solar energy exhibits unique advantages when applied for water purification, desalination, high-temperature heterogeneous catalysis, anti-bacterial treatments, and deicing. In this review, the various photothermal conversion mechanisms based on different forms of heat release are summarized and some of the latest examples are presented. In addition, the necessary prerequisites for solar-driven photothermal materials toward their practical applications are also discussed. Further, the latest advances in photothermal conversion of solar energy are discussed, focusing on different types of photothermal applications. Finally, a summary is given and the challenges and opportunities in the photothermal conversion of solar energy are presented. This review aims to give a comprehensive understanding of emerging solar energy conversion technologies based on the photothermal effect, especially by using nanomaterials and nanostructures.



https://doi.org/10.1002/adsu.202200115
Li, Yuhang; Wang, Dong; Liang, Zhengchen; Zeng, Lingxiao; Li, Wenxue; Xie, Peng; Ding, Qi; Zhang, Hong; Schaaf, Peter; Wang, Wei
Evaluating the optical response of heavily decorated black silicon based on a realistic 3D modeling methodology. - In: ACS applied materials & interfaces, ISSN 1944-8252, Bd. 14 (2022), 31, S. 36189-36199

Combining black silicon (BS), a nanostructured silicon containing highly roughened surface morphology with plasmonic materials, is becoming an attractive approach for greatly enhancing light-matter interactions with promising applications of sensing and light harvesting. However, precisely describing the optical response of a heavily decorated BS structure is still challenging due to the increasing complexity in surface morphology and plasmon hybridization. Here, we propose and fully characterize BS-based multistacked nanostructures with randomly distributed nanoparticles on the highly roughened nonflat surface. We demonstrate a realistic 3D modeling methodology based on parametrized scanning electron microscopy images that provides high-precision morphology details, successfully linking the theoretical analysis with experimental optical response of the complex nanostructures. Far-field calculations very nicely reproduce experimental reflectance spectra, revealing the dependency of light trapping on the thickness of the conformal reflector and the atop nanoparticle size. Near-field analysis clearly identifies three types of stochastic “hotspots”. Their contribution to the overall field enhancement is shown to be very much sensitive to the nanoscale surface morphology. The simulated near-field property is then used to examine the measured surface-enhanced Raman scattering (SERS) response on the multistacked structures. The present modeling approach combined with spectroscopic characterizations is expected to offer a powerful tool for the precise description of the optical response of other large-scale highly disordered realistic 3D systems.



https://doi.org/10.1021/acsami.2c05652