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磁场效应(magnetic field effects, MFEs)指的是材料或器件的光电物理特性(包括光致发光、电致发光、注入电流、光电流等)在外加磁场下发生的变化. 本文所述的是非磁性发光材料的MFEs, 其首先在有机半导体光电器件中被发现. 近十几年来, MFEs作为一种新兴的物理现象引起了广泛的研究; 同时它也成为一种独特的实验手段, 用以探讨有机半导体中电荷的输运、复合以及自旋极化等过程. 近期的研究发现, MFEs不仅存在于有机半导体中, 而且在拥有强自旋-轨道耦合作用的金属卤化物钙钛矿材料中被观测到, 这既拓展了MFEs的研究方向, 也为通过研究MFEs来探索金属卤化物钙钛矿器件的物理机制, 进而为提升其器件性能提供了契机. 本文重点关注有机半导体和卤化物钙钛矿在磁场下的电致发光和光致发光变化, 即发光的磁场效应. 回顾了到目前为止主流的理论模型和代表性实验现象, 对比分析了磁场下有机半导体和卤化物钙钛矿的发光物理行为. 以期为有机及钙钛矿磁场效应领域的研究提供一些思路, 同时为有机及钙钛矿发光领域的发展贡献些许想法.Magnetic field effects (MFEs) are used to describe the changes of the photophysical properties (including photoluminescence, electroluminescence, injectedcurrent, photocurrent, etc.) when materials and devices are subjected to the external magnetic field. The MFEs in non-magnetic luminescent materials and devices were first observed in organic semiconductor. In the past two decades, the effects have been studied extensively as an emerging physical phenomenon, and also used as a unique experimental method to explore the processes such as charge transport, carrier recombination, and spin polarization in organic semiconductors. Recent studies have found that the MFEs can also be observed in metal halide perovskites with strong spin-orbital coupling. Besides, for expanding the research domain of MFEs, these findings can also be utilized to study the physical mechanism in metal halide perovskites, and then provide an insight into the improving of the performance of perovskite devices. In this review, we focus on the magnetic field effects on the electroluminescence and photoluminescence changes of organic semiconductors and halide perovskites. We review the mainstream of theoretical models and representative experimental phenomena which have been found to date, and comparatively analyze the luminescence behaviors of organic semiconductors and halide perovskites under magnetic fields. It is expected that this review can provide some ideas for the research on the MFEs of organic semiconductors and halideperovskites, and contribute to the research of luminescence in organic materials and halideperovskites.
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Keywords:
- organic semiconductors /
- halide perovskites /
- light-emitting devices /
- magnetic field effects
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图 2 Alq3器件在不同电压下的(a) MC和(b) MEL[13]; (c) Ru(bpy)3器件在不同电压下的MEL[12]; (d)不同长度一维结构器件的MR[20]; 延迟荧光器件在不同温度下的(e) MC和(f) MEL[21]
Fig. 2. The (a) MC and (b) MEL of Alq3-based OLED at different voltages[13]; (c) the MEL of Ru(bpy)3-based OLED at different voltages[12]; (d) the MR in the device with one-dimensional structure[20]; the (e) MC and (f) MEL of delayed fluorescence OLED at different temperatures [21] .
图 4 (a)自由载流子、电子-空穴对和激子的跃迁能级示意图及相关速率常数, 其中S和T分别表示单线态和三线态, G表示EHP的形成率,
$ {k}_{\mathrm{d}}^{\mathrm{S}} $ 和$ {k}_{\mathrm{d}}^{\mathrm{T}} $ 分别代表单线态和三线态EHP的离解速率常数,$ {k}_{\mathrm{r}}^{\mathrm{S}} $ 和$ {k}_{\mathrm{r}}^{\mathrm{T}} $ 为单线态和三线态EHP的复合速率常数; (b)电子、空穴在磁场下以不同频率$ \omega $ 进动示意图Fig. 4. (a) Transition rate constants of free carriers, electron-hole pairs and excitons. S and T represent singlet and triplet states, respectively. G represents the formation rate of EHP.
$ {k}_{\mathrm{d}}^{\mathrm{S}} $ and$ {k}_{\mathrm{d}}^{\mathrm{T}} $ represent the dissociation rate constants of singlet and triplet EHPs, respectively,$ {k}_{\mathrm{r}}^{\mathrm{S}} $ and$ {k}_{\mathrm{r}}^{\mathrm{T}} $ are the recombination rate constants of singlet and triplet EHPs. (b) The Larmor precession of electrons and holes with different frequency ω under a magnetic field.
图 11 (a)电子-空穴对中Δg机制示意图; (b) 5 mA恒定电流下的MEL; (c)钙钛矿薄膜的MPL; (d) 0和5 T磁场下左右圆偏振旋光光谱; (e) 18 K温度下薄膜的圆偏振度与磁场的关系[35]
Fig. 11. (a) Schematic diagram of the Δg mechanism of electron-hole pairs; (b) the MEL at a constant current of 5 mA; (c) the MPL of the perovskite film; (d) the left and right circularly polarized optical rotation spectra at 0 and 5 T; (e) the relationship between the degree of circularly polarization and the magnetic field at 18 K [35] .
图 12 (a)钙钛矿薄膜在不同激发光强下的MPL; (b)钙钛矿光伏器件在不同激发光强下的MC; (c)正MC和负MPL的线形特征; (d)钙钛矿中的电子-空穴对模型示意图[33]
Fig. 12. (a) MPL of the perovskite film with different excitation intensities at room temperature; (b) MC of the perovskite solar cell with different excitation intensities; (c) linear characteristics of positive MC and negative MPL; (d) schematic diagram of the electron-hole pair model in perovskites [33] .
图 13 (a) (C4H9NH3)2PbBr4的PL谱, 其中Γ1和Γ2为暗态, Γ5为亮态; (b)自旋驰豫(左图)和自旋翻转(右图)示意图; (c) PL随磁场的变化[32]
Fig. 13. (a) PL spectra of (C4H9NH3)2PbBr4, where Γ1 and Γ2 are dark states, and Γ5 is bright state; (b) schematic diagram of the spin relaxation (left) and spin flip (right); (c) the PL changes under the magnetic fields[32] .
图 14 (a) 0 ℃下, CsPbBr3薄膜有/无500 mT的PL光谱; (b)无磁场和(c)有磁场的瞬态PL光谱; (d)无磁场和(e)有磁场下515 nm处复合动力学轨迹[34]
Fig. 14. (a) The PL spectra of CsPbBr3 film with/without a magnetic field of 500 mT at 0 ℃; the time resolved PL spectra in the obsence (b) and presence (c) of a magnetic field; the recombination kinetics extracted from the time resolved PLs in the obsence (d) and presence (e) of a magnetic field [34].
Power/(mW· cm–2) Magnet OFF Magnet ON Fast decay/ps Slow decay/ps Fast decay/ps Slow decay/ps 198 138$ \pm $9 (55%) 1038$ \pm $65 (45%) 104$ \pm $6 (63%) 959$ \pm $55 (37%) 305 138$ \pm $8 (55%) 1031$ \pm $31 (45%) 100$ \pm $4 (64%) 886$ \pm $25 (36%) 450 131$ \pm $5 (57%) 1000$ \pm $34 (43%) 101$ \pm $5 (65%) 892$ \pm $23 (35%) 
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