TY  - JOUR
A1  - Weissenseel, Sebastian
A1  - Gottscholl, Andreas
A1  - Bönnighausen, Rebecca
A1  - Dyakonov, Vladimir
A1  - Sperlich, Andreas
T1  - Long-lived spin-polarized intermolecular exciplex states in thermally activated delayed fluorescence-based organic light-emitting diodes
JF  - Science Advances
N2  - Spin-spin interactions in organic light-emitting diodes (OLEDs) based on thermally activated delayed fluorescence (TADF) are pivotal because radiative recombination is largely determined by triplet-to-singlet conversion, also called reverse intersystem crossing (RISC). To explore the underlying process, we apply a spin-resonance spectral hole-burning technique to probe electroluminescence. We find that the triplet exciplex states in OLEDs are highly spin-polarized and show that these states can be decoupled from the heterogeneous nuclear environment as a source of spin dephasing and can even be coherently manipulated on a spin-spin relaxation time scale T-2* of 30 ns. Crucially, we obtain the characteristic triplet exciplex spin-lattice relaxation time T-1 in the range of 50 mu s, which far exceeds the RISC time. We conclude that slow spin relaxation rather than RISC is an efficiency-limiting step for intermolecular donor:acceptor systems. Finding TADF emitters with faster spin relaxation will benefit this type of TADF OLEDs.
KW  - detected magnetic-resonance
KW  - population oscillations
KW  - polaron delocalization
KW  - charge separation
KW  - hole
KW  - phosphorescence
KW  - singlet
KW  - absorption
KW  - tryptophan
KW  - emission
Y1  - 2021
U6  - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:bvb:20-opus-265508
VL  - 7
IS  - 47
ER  - 
TY  - JOUR
A1  - Gottscholl, Andreas
A1  - Wagenhöfer, Maximilian
A1  - Klimmer, Manuel
A1  - Scherbel, Selina
A1  - Kasper, Christian
A1  - Baianov, Valentin
A1  - Astakhov, Georgy V.
A1  - Dyakonov, Vladimir
A1  - Sperlich, Andreas
T1  - Superradiance of spin defects in silicon carbide for maser applications
JF  - Frontiers in Photonics
N2  - Masers as telecommunication amplifiers have been known for decades, yet their application is strongly limited due to extreme operating conditions requiring vacuum techniques and cryogenic temperatures. Recently, a new generation of masers has been invented based on optically pumped spin states in pentacene and diamond. In this study, we pave the way for masers based on spin S = 3/2 silicon vacancy (V\(_{Si}\)) defects in silicon carbide (SiC) to overcome the microwave generation threshold and discuss the advantages of this highly developed spin hosting material. To achieve population inversion, we optically pump the V\(_{Si}\) into their m\(_S\) = ±1/2 spin sub-states and additionally tune the Zeeman energy splitting by applying an external magnetic field. In this way, the prerequisites for stimulated emission by means of resonant microwaves in the 10 GHz range are fulfilled. On the way to realising a maser, we were able to systematically solve a series of subtasks that improved the underlying relevant physical parameters of the SiC samples. Among others, we investigated the pump efficiency as a function of the optical excitation wavelength and the angle between the magnetic field and the defect symmetry axis in order to boost the population inversion factor, a key figure of merit for the targeted microwave oscillator. Furthermore, we developed a high-Q sapphire microwave resonator (Q ≈ 10\(^4\)–10\(^5\)) with which we find superradiant stimulated microwave emission. In summary, SiC with optimized spin defect density and thus spin relaxation rates is well on its way of becoming a suitable maser gain material with wide-ranging applications.
KW  - stimulated emission
KW  - maser
KW  - population inversion
KW  - silicon vacancy
KW  - spin polarization
KW  - superradiance
Y1  - 2022
U6  - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:bvb:20-opus-284698
SN  - 2673-6853
VL  - 3
ER  - 
TY  - JOUR
A1  - Gottscholl, Andreas
A1  - Diez, Matthias
A1  - Soltamov, Victor
A1  - Kasper, Christian
A1  - Krauße, Dominik
A1  - Sperlich, Andreas
A1  - Kianinia, Mehran
A1  - Bradac, Carlo
A1  - Aharonovich, Igor
A1  - Dyakonov, Vladimir
T1  - Spin defects in hBN as promising temperature, pressure and magnetic field quantum sensors
JF  - Nature Communications
N2  - Spin defects in solid-state materials are strong candidate systems for quantum information technology and sensing applications. Here we explore in details the recently discovered negatively charged boron vacancies (V\(_B\)\(^−\)) in hexagonal boron nitride (hBN) and demonstrate their use as atomic scale sensors for temperature, magnetic fields and externally applied pressure. These applications are possible due to the high-spin triplet ground state and bright spin-dependent photoluminescence of the V\(_B\)\(^−\). Specifically, we find that the frequency shift in optically detected magnetic resonance measurements is not only sensitive to static magnetic fields, but also to temperature and pressure changes which we relate to crystal lattice parameters. We show that spin-rich hBN films are potentially applicable as intrinsic sensors in heterostructures made of functionalized 2D materials.
KW  - electronic properties and materials
KW  - qubits
Y1  - 2021
U6  - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:bvb:20-opus-261581
VL  - 12
IS  - 1
ER  -