RESUMEN
Chiral lead halide perovskites (LHPs) have been widely investigated in chiroptical spintronics due to their significant Rashba spin-orbit coupling (SOC) and chiral-induced spin selectivity (CISS). Ferromagnet/LHP spinterface stems from the orbital hybridization at the interface of the ferromagnet and the nonmagnetic semiconductor, where interfacial density of state is spin-dependent. By far, the impact of the ferromagnet/chiral LHP spinterface on magneto-photoluminescence (Magneto-PL) of chiral LHPs remains unknown. In this work, we find that the negative and tunable Magneto-PL effects for the pristine LHP bulk film can be drastically enhanced by incorporating ferromagnetic/chiral LHP interfaces. A large Magneto-PL magnitude can reach approximately -13% for the Ni/(S-MBA)2PbI4 interface at the field strengths of ±900 mT. With the assistance of circularly polarized PL spectra, anisotropic magneto-resistance, and X-ray photoelectron spectroscopy measurements, we demonstrate that the ferromagnet/chiral LHP interfaces are chirality/spin-dependent and possess ferromagnetic property due to distinct magnetic switching behavior and electronic orbit coupling at interfaces, which boost the Rashba splitting and spin mixing. The comprehensive effects of Rashba-induced exciton states and chiral-induced SOC at chiral spinterfaces with CISS are responsible for the enhanced Magneto-PL of Ni/(R/S-MBA)2PbI4. It is postulated that the chiral spinterfaces play a dominant role for achieving large and tunable magneto-optical effect of chiral LHPs. This work paves the way for chiroptical spintronic applications.
RESUMEN
Low-temperature solution-made chiral lead halide perovskites (LHPs) have spontaneous Bychkov-Rashba spin orbit coupling (SOC) and chiral-induced spin selectivity (CISS) qualities. Their coexistence may give rise to considerable spin and charge conversion capabilities for spin-orbitronic applications. In this study, we demonstrate the spin-photogalvanic effect for (R-MBA)2PbI4 and (S-MBA)2PbI4 polycrystalline film-based lateral devices (100 µm channel length). The light helicity dependence of the short-circuit photocurrent exhibits the circular photogalvanic effect (CPGE) and linear photogalvanic effect (LPGE) with decent two-fold symmetry for a complete cycle in a wide temperature range from 4 K to 300 K. Because of the Rashba SOC and the material helicity, the effect is converse for the two chiral LHPs. In addition, its magnitude and sign can be effectively tuned by constant magnetic fields. The Rashba effect, CISS-generated unbalanced spin transport, and chiral-induced magnetization are mutually responsible for it. Our study evidently proves the future prospect of using chiral LHPs for spin-orbitronics.
RESUMEN
The introduction of chiral organic ligands into hybrid organic-inorganic perovskites (HOIPs) results in chiral perovskites, which exhibit natural optical activities (NOAs) such as circularly polarized luminescence (CPL). CPL can be observed in achiral HOIPs under a magnetic field as well. Here, we systematically study the temperature- and magnetic field-dependence of both circular polarization and total intensity in chiral HOIPs. Pronounced CPL polarization is observed in polycrystalline films of chiral HOIPs, which can be further tuned by an applied magnetic field. The magnetic field also modifies the total intensity of CPL, giving rise to magneto-PL in chiral HOIPs, which is observable even at room temperature. The observed field and temperature-dependence of polarization can be well accounted for by a recently developed theory of chiral HOIPs, where the materials' helicity gives rise to a novel spin-orbit coupling (SOC). The observed MPL can be quantitatively accounted for by the interplay of exciton fine structures and the magnetic field. Our study suggests that the magnetic field provides an effective means to manipulate both the polarization and intensity of CPL in chiral HOIPs, which can be exploited for novel device applications.
RESUMEN
Using the fingerprint magneto-electroluminescence trace, we observe a fascinating high-level reverse intersystem crossing (HL-RISC) in rubrene-doped organic light-emitting diodes (OLEDs). This HL-RISC is achieved from high-lying triplet states (T2,rub) transferred from host triplet states by the Dexter energy transfer to the lowest singlet states (S1,rub) in rubrene. Although HL-RISC decreases with bias current, it increases with lowering temperature. This is contrary to the temperature-dependent RISC from conventional thermally activated delayed fluorescence, because HL-RISC is an exothermic process instead. Moreover, owing to the competition of exciton energy transfer with direct charge trap, HL-RISC changes nonmonotonically with the dopant concentration and increases luminous efficiency to a maximum at 10% of rubrene, which is about ten times greater than that from the pure-rubrene device. Additionally, the HL-RISC process is not observed in bare rubrene-doped films because of the absence of T2,rub. Our findings pave the way for designing highly efficient orange fluorescent OLEDs.
RESUMEN
The thermally activated delayed fluorescence (TADF) material 2,3,5,6-tetrakis(3,6-diphenylcarbazol-9-yl)-1,4-dicyanobenzene (4CzTPN-Ph) and the conventional fluorescent dopant 4-(dicyanomethylene)-2-tert-butyl-6-(1,1,7,7-tetramethyljulolidin-4-yl-vinyl)-4H-pyran (DCJTB) were used to co-dope the host material 4,4'-bis(carbazol-9-yl)biphenyl (CBP) for the fabrication of TADF-assisted fluorescent organic light-emitting diodes (OLEDs). Some exceptional magnetic field effect (MFE) curves with abundant structures and four tunable components within a low magnetic field range (≤50 mT) were obtained, in sharp contrast to the maximum of two components observed in typical OLEDs. These MFE components were easily tuned by the injection current, dopant concentration, working temperature, and dopant energy gap, leading to a wide variety of MFE curve line shapes. The experimental results are attributed to the spin-pair state inter-conversions occurring in the device, including intersystem crossing (ISC) of CBP polaron pairs, ISC of 4CzTPN-Ph polaron pairs, reverse ISC (RISC) of 4CzTPN-Ph excitons, RISC of DCJTB polaron pairs, DCJTB triplet fusion, and DCJTB triplet-charge annihilation. Moreover, the exciton energy transfer processes among the host material and the guest dopants had a pronounced impact on the formation of these four components. This work gives a deeper understanding of the microscopic mechanisms of TADF-based co-doped systems for the further development of organic magnetic field effects in the extensive field of OLEDs.
RESUMEN
Singlet fission is usually the only reaction channel for excited states in rubrene-based organic light-emitting diodes (OLEDs) at ambient temperature. Intriguingly, we discover that triplet fusion (TF) and intersystem crossing (ISC) within rubrene-based devices begin at moderate and high current densities (j), respectively. Both processes enhance with decreasing temperature. This behavior is discovered by analyzing the magneto-electroluminescence curves of the devices. The j-dependent magneto-conductance, measured at ambient temperature indicates that spin mixing within polaron pairs that are generated by triplet-charge annihilation (TQA) causes the occurrence of ISC, while the high concentrations of triplets are responsible for generating TF. Additionally, the reduction in exciton formation and the elevated TQA with decreasing temperature may contribute to the enhanced ISC at low temperatures. This work provides considerable insight into the different mechanisms that occur when a high density of excited states exist in rubrene and reasonable reasons for the absence of EL efficiency roll-off in rubrene-based OLEDs.
