CRC 951/3: Hybrid Inorganic/Organic Systems (HIOS) for Opto-Electronics

The ability to precisely control the formation of heterostructures from different materials has revolutionized electronic and optical technologies during the past decades. However, tackling the increasing challenges faced by these key technologies requires radically new approaches. In this spirit, the CRC has launched a both ground breaking and comprehensive research programme combining three significantly different classes of materials in hybrid inorganic/organic systems (HIOS) with the aim of realizing substantially improved and potentially novel opto-electronic functionalities: inorganic semiconductors feature high charge carrier mobilities, conjugated organic molecules exhibit strong light-matter coupling, while metal nanostructures excel at confining and guiding light at subwavelength dimensions. Each material class can conceivably contribute unique properties, and their merger had not been systematically attempted. For fully harnessing this potential, the CRC elucidated the fundamental chemical, electronic, photonic, and plasmonic interactions arising from the different nature of the components combined in HIOS, and uncovered novel hybridized quantum states and coupled excitations at their interfaces. In hand with this, we comprehended the limitations of state-of-the-art bulk inorganic semiconductors for achieving intimate coupling with conjugated molecules. Due to ubiquitous surface states and band bending from the surface into the semiconductor bulk, a passive interlayer compromises functionality.In the upcoming funding period, we will exploit the extremely high surface-to-volume ratio and strong light-matter interaction of atomically thin transition metal dichalcogenide monolayers, which emerged during the second funding period as ideal inorganic semiconductor component for the goals of the CRC. These monolayers feature superior structural quality and stability compared to previously used semiconductors. The fact that we can now realise HIOS that are comprised of the active region only, i.e., the interface, provides novel opportunities that were not realistically imaginable before. We now set out to achieve ultimate coupling and functionality. Furthermore, because we have access to nanometre thin, interface-only HIOS we can unleash the full potential of metal nanostructures for plasmonic enhancement of light absorption and emission by several orders of magnitude. Combined with new generations of our unique molecular photoswitches, the extensive know-how gathered within the CRC 951 enables us to realise advanced HIOS that will pave the way for unequalled nanoscale solid-state devices, not achievable with any of the individual material classes alone. Now within reach, these ultra-compact devices will feature superior functionality, such as high modulation frequency light emission and sensing, widely tuneable quantum emission, chirality sensing, electronic and optical multi-functionality, and even synapse and neuron emulation.

Principal Investigators
Koch, Norbert Prof. Dr. techn. (Details) (Structure, Dynamics and electronic Properties of Molecular Systems)

Duration of Project
Start date: 07/2019
End date: 06/2023

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Research Areas
Experimental Condensed Matter Physics, Natural Sciences, Optics, Quantum Optics and Physics of Atoms, Molecules and Plasmas

Research Areas
Experimentelle Physik, kondensierte Materie, Festkörperphysik, Materialwissenschaften, Oberflächenphysik, Optik, Organische Chemie, Photonik, Physikalische Chemie, Physik molekularer Systeme, Theoretische Physik

2020 (stand 3. März)

G. Ligorio, G. F. Cotella, A. Bonasera, N. Zorn Morales, G. Carnicella, B. Kobin, Q. Wang, N. Koch, S. Hecht, E. J.W. List-Kratochvil, F. Cacialli
Modulating the luminance of organic light-emitting diodes via optical stimulation of a photochromic molecular monolayer at transparent oxide electrode
Nanoscale (2020)
doi: 10.1039/D0NR00724B

L. Grill, S. Hecht
Covalent on-surface polymerization
Nat. Chem. 12, 115 (2020)
doi: 10.1038/s41557-019-0392-9

H. Qiu, Z. Liu, Y. Yao, M. Herder, S. Hecht, P. Samorì
Simultaneous optical tuning of hole and electron transport in ambipolar WSe2 interfaced with a bicomponent photochromic layer: From high-mobility transistors to flexible multilevel memories
Adv. Mater. 1907903 (2020)
doi: 10.1002/adma.201907903

F. Caruso, D. Novko, C. Draxl
Photoemission signatures of nonequilibrium carrier dynamics from first principles
Phys. Rev. B 101 035128 (2020)
doi: 10.1103/PhysRevB.101.035128

M. Raoufi, U. Hörmann, G. Ligorio, J. Hildebrandt, M. Pätzel, E. List-Kratochvil, S. Hecht, D. Neher
Simultaneous effect of UV-radiation and surface modification on the work function and hole injection properties of ZnO thin films
Phys. Status Solidi A 1900876 (2020)
doi: 10.1002/pssa.201900876

N. Mutz, S. Park, T. Schultz, S. Sadofev, S, Dalgleish, L. Reissig, N. Koch, E. J. W. List-Kratochvil, S. Blumstengel
Excited-State Charge Transfer Enabling MoS2/Phthalocyanine Photodetectors with Extended Spectral Sensitivity
J. Phys. Chem. C 124, 2837 (2020)
doi: 10.1021/acs.jpcc.9b10877

D. Reiche, K. Busch, F. Intravaia
Quantum thermodynamics of overdamped modes in local and spatially dispersive materials
Phys. Rev. A 101, 012506 (2020)
doi: 10.1103/PhysRevA.101.012506

C. M. Wolff, L. Canil, C. Rehermann, N. L. Nguyen, F. Zu, M. Ralaiarisoa, P. Caprioglio, L. Fiedler ,M. Stolterfoht, S. Kogikoski Jr., I. Bald, N. Koch, E. L. Unger, T. Dittrich, A. Abate, D. Neher
Perfluorinated self-assembled monolayers enhance the stability and efficiency of inverted perovskite solar cells
ACS Nano (2020)
doi: 10.1021/acsnano.9b03268

J. Hu, N. Aghdassi, Y. Garmshausen, M. Oehzelt, R. Wang, N. Koch, S. Hecht, S. Duhm, I. Salzmann
Dipolar Substitution Impacts Growth and Electronic Properties of para-Sexiphenyl Thin Films
Adv. Funct. Mater. 7, 1903440 (2020)
doi: 10.1002/admi.201901707

A. J. Ramadan, M. Ralaiarisoa, F. Zu, L. A. Rochford, B. Wenger, N. Koch, H. J. Snaith
Revealing the stoichiometric tolerance of lead trihalide perovskite thin films
Chem. Mater. 32, 114 (2020)
doi: 10.1021/acs.chemmater.9b02639

W. Rekab, T. Leydecker, L. Hou, H. Chen, M. Kirkus, C. Cendra, M. Herder, S. Hecht, A. Salleo, I. Mc Culloch, E. Orgiu, P. Samorí
Phototuning selectively hole and electron transport in optically switchable ambipolar transistors
Adv. Funct. Mater. 30, 1908944 (2020)
doi: 10.1002/adfm.201908944

R. Wang, Y. Wang, C. Wu, T. Zhai, J. Yang, B. Sun, S. Duhm, N. Koch
Direct observation of conductive polymer induced inversion layer in n‐Si and correlation to solar cell performance
Adv. Funct. Mater. 30, 1901707 (2020)
doi: 10.1002/adfm.201903440

G. Reecht, N. Krane, C. Lotze, L. Zhang, A. L. Briseno, K. J. Franke
Vibrational excitation mechanism in tunneling spectroscopy beyond the Franck-Condon model
arXiv: 2001.10499

2019 (ab Juli)

C. H. Egerland, K. Busch, F. Intravaia
Polaritonic contribution to the Casimir energy between two graphene layers
Phys. Rev. B 100, 235418 (2019)
doi: 10.1103/PhysRevB.100.235418

P. Storm, M. Kneiß, A. Hassa, T. Schultz, D. Splith, H. von Wenckstern, N. Koch, M. Lorenz, M. Grundmann
Epitaxial κ-(AlxGa1−x)2O3 thin films and heterostructures grown by tin-assisted VCCS-PLD
APL Mater. 7, 111110 (2019)
doi: 10.1063/1.5124231

M. Carroli, D. T. Duong, E. Buchaca Domingo, A. Liscio, K. Börjesson, M. Herder, V. Palermo, S. Hecht, N. Stingelin, A. Salleo, E. Orgiu,* P. Samorì
The role of morphology in optically switchable transistors based on a photochromic molecule / p-type polymer semiconductor blend
Adv. Funct. Mater. 1907507 (2019)
doi: 10.1002/adfm.201907507

D. Christiansen, M. Selig, E. Malic, R. Ernstorfer, A. Knorr
Theory of exciton dynamics in time-resolved ARPES: Intra- and intervalley scattering in two-dimensional semiconductors
Phys. Rev. B 100, 205401 (2019)
doi: 10.1103/PhysRevB.100.205401

S. Mei, Z. Kochovski, R. Roa, S. Gu, X. Xu, H. Yu, J. Dzubiella, M. Ballauff, Y. Lu
Enhanced Catalytic Activity of Gold@Polydopamine Nanoreactors with Multi-compartment Structure Under NIR Irradiation
Nano-Micro Letters 11, 83 (2019)
doi: 10.1007/s40820-019-0314-9

B. Wegner, L. Grubert, D. Chercka, A. Opitz, A. Röttger, Y. Zhang, S. Barlow, S. R. Marder, S. Hecht, K. Müllen, N. Koch
Predicting the yield of ion pair formation in molecular electrical doping: redox-potentials versus ionization energy/electron affinity
J. Mater. Chem. C 7, 13839 (2019)
doi: 10.1039/C9TC04500G

M. Selig, F. Katsch, S. Brem, G. F. Mkrtchian, E. Malic, A. Knorr
Quenching of Intervalley Exchange Coupling in the Presence of Momentum-Dark States in TMDCs
arXiv: 1908.11178v1

S. Brem, A. Ekman, D. Christiansen, F. Katsch, M. Selig, C. Robert, X. Marie, B. Urbaszek, A. Knorr, E. Malic
Phonon-assisted Photoluminescence from Dark Excitons in Monolayers of Transition Metal Dichalcogenides
arXiv: 1904.04711v1

J. Ren, S. Franke, A. Knorr, M. Richter, S. Hughes
Efficient near-field to far-field transformations for quasinormal modes of optical cavities and plasmonic resonators
arXiv: 1912.08309

J. Kim, A. Gulans, C. Draxl
Work-function modification of PEG(thiol) adsorbed on the Au(111) surface: A first-principles study
arXiv: 1911.12165

M. Selig, F. Katsch, R. Schmidt, S. Michaelis de Vasconcellos, R. Bratschitsch, E. Malic, A. Knorr
Ultrafast dynamics in monolayer transition metal dichalcogenides: Interplay of dark excitons, phonons, and intervalley exchange
Phys. Rev. Research 1, 022007(R) (2019)
doi: 10.1103/PhysRevResearch.1.022007

F. Intravaia, M. Oelschläger, D. Reiche, D. A. R. Dalvit, and K. Busch
Quantum Rolling Friction
Phys. Rev. Lett. 123, 120401 (2019)
doi: 10.1103/PhysRevLett.123.120401

S. Park, T. Schultz, X. Xu, B. Wegner, A. Aljarb, A. Han, L.-J. Li, V. C. Tung, P. Amsalem, N. Koch
Demonstration of the key substrate-dependent charge transfer mechanisms between monolayer MoS2 and molecular dopants
Communications Physics 2, 109 (2019)
doi: 10.1038/s42005-019-0212-y

G. F. Mkrtchian, A. Knorr, M. Selig
Theory of second-order excitonic nonlinearities in transition metal dichalcogenides
Phys. Rev. B 100, 125401 (2019)
doi: 10.1103/PhysRevB.100.125401

D. Nabok, B. Höffling, C. Draxl
Energy-Level Alignment at Organic/Inorganic Interfaces from First Principles: Example of Poly(para-phenylene)/Rock-Salt ZnO(100)
Chem. Mater. 31, 7143 (2019)
doi: 10.1021/acs.chemmater.9b01802

C. Vorwerk, B. Aurich, C. Cocchi, C. Draxl
Bethe-Salpeter equation for absorption and scattering spectroscopy: Implementation in the "exciting" code
Electron. Struct. 1, 037001 (2019)
doi: 10.1088/2516-1075/ab3123

S. Vempati, L. Bogner, C. Richter, J.-C. Deinert, L. Foglia, L. Gierster, J. Stähler
Photoexcited organic molecules en route to highly efficient autoionization
arXiv: 1911.04333

V. C. Nikolis, A. Mischok, B. Siegmund, J. Kublitski, X. Jia, J. Benduhn, U. Hörmann, D. Neher, M. C. Gather, D. Spoltore, K. Vandewal
Strong light-matter coupling for reduced photon energy losses in organic photovoltaics
Nature Communications 10, 3706 (2019)
doi: 10.1038/s41467-019-11717-5

H. Qiu, Y. Zhao, Z. Liu, M. Herder, S. Hecht, P. Samorì
Modulating the charge transport in two-dimensional semiconductors via energy level phototuning
Adv. Mater. 31, 1903402 (2019)
doi: 10.1002/adma.201903402

A. Eljarrat, C. T. Koch
Design and application of a relativistic Kramers-Kronig analysis algorithm
Ultramicroscopy 206, 112825 (2019)
doi: 10.1016/j.ultramic.2019.112825

P. Caprioglio, M. Stolterfoht, C. M. Wolff, T. Unold, B. Rech, S. Albrecht, D. Neher
On the Relation between the Open‐Circuit Voltage and Quasi‐Fermi Level Splitting in Efficient Perovskite Solar Cells
Advanced Energy Materials 9, 1901631 (2019)
doi: 10.1002/aenm.201901631

M. Stolterfoht, P. Caprioglio, C. M. Wolff, J. A. Márquez, J. Nordmann, S. Zhang, D. Rothhardt, U. Hörmann, A. Redinger, L. Kegelmann, S. Albrecht, T. Kirchartz, M. Saliba, T. Unold, D. Neher
The impact of energy alignment and interfacial recombination on the internal and external open-circuit voltage of perovskite solar cells
Energy Environ. Sci. 12, 2778 (2019)
doi: 10.1039/c9ee02020a

S. Hughes, S. Franke, C. Gustin, M. K. Dezfouli, A. Knorr, M. Richter
Theory and Limits of On-Demand Single-Photon Sources Using Plasmonic Resonators: A Quantized Quasinormal Mode Approach
ACS Photonics 6, 2168 (2019)
doi: 10.1021/acsphotonics.9b00849

R. Schlesinger, F. Bussolotti, J. Yang, S. Sadofev, A. Vollmer, S. Blumstengel, S. Kera, N. Ueno, N. Koch
Gap states induce soft Fermi level pinning upon charge transfer at ZnO/molecular acceptor interfaces
Phys. Rev. Materials 3, 074601 (2019)
doi: 10.1103/PhysRevMaterials.3.074601

S. Caicedo-Dávila, H. Funk, R. Lovrinčić, C. Müller, M. Sendner, O. Cojocaru-Mirédin, F. Lehmann, R. Gunder, A, Franz, S, Levcenco, A. V. Cohen, L. Kronik, B. Haas, C. T. Koch, D. Abou-Ras
Spatial Phase Distributions in Solution-Based and Evaporated Cs–Pb–Br Thin Films
J. Phys. Chem. C 123, 17666 (2019)
doi: 10.1021/acs.jpcc.9b02567

K.-W. Lau, C. Cocchi, C. Draxl
Electronic and optical excitations of two-dimensional ZrS2 and HfS2 and their heterostructure
Phys. Rev. Materials 3, 074001 (2019)
doi: 10.1103/PhysRevMaterials.3.074001

Last updated on 2021-28-07 at 09:41