Spin-Dependent Photovoltaic and Photogalvanic Responses of Optoelectronic Devices Based on Chiral Two-Dimensional Hybrid Organic–Inorganic Perovskites

Abstract

Two-dimensional hybrid organic−inorganic perovskites (2D-HOIPs) that form natural multiple quantum wells have attracted increased research interest due to their interesting physics and potential applications in optoelectronic devices. Recent studies have shown that spintronics applications can also be introduced to 2D-HOIPs upon integrating chiral organic ligands into the organic layers. Here we report spin-dependent photovoltaic and photogalvanic responses of optoelectronic devices based on chiral 2D-HOIPs, namely, (R-MBA) 2 PbI 4 and (S-MBA) 2 PbI 4 . The out-of-plane photocurrent response in vertical photovoltaic devices exhibits ∼10% difference upon right and left circularly polarized light (CPL) excitation, which originates from selective spin transport through the chiral multilayers. In contrast, the in-plane photocurrent response generated by CPL excitation of planar photoconductive devices shows a typical response of chirality-induced circular photogalvanic effect that originates from the Rashba splitting in the electronic bands of these compounds. Our studies may lead to potential applications of chiral 2D-HOIPs in optoelectronic devices that are sensitive to the light helicity.

Chirality‐Dependent Circular Photogalvanic Effect in Enantiomorphic 2D Organic–Inorganic Hybrid Perovskites

“…In a very recent report, we found that the CPGE has been observed in another 2D-OIHP lead(II) iodide with introduced chiral molecules. [54] However, the photocurrent measurement of that report was conducted in a different configuration from our study, where the in-plane light propagation vector is nearly perpendicular to the photocurrent direction. In such configuration, the observed CPGE photocurrent would originate predominantly from the polarity at the sample surface rather than chirality of bulk crystal (Scheme S3c,d, Supporting Information) as reported in centrosymmetric OIHP/2D-OIHP lead(II) halides.…”

Structural descriptor for enhanced spin-splitting in 2D hybrid perovskites

“…When such distortions break the inversion symmetry of the inorganic layer, Rashba/Dresselhaus spin-splitting can emerge due to spin-orbit coupling (SOC) [20][21][22][23][24] . Rashba/Dresselhaus spinsplitting is a relativistic quantum phenomenon in condensed matter that leads to important physical manifestations for emerging spin-orbitronic devices, including intrinsic spin-Hall effect 25 , gate-controlled spin precession 26 , (inverse) spin galvanic effects, photogalvanic effects 27 , and chiroptic effects 28 , that rely on SOC-mediated manipulation of the spin degrees of freedom by electrical, optical, or magnetic means 22,25 .…”

Heterogeneous Integration of Chiral Lead–Chloride Perovskite Crystals with Si Wafer for Boosted Circularly Polarized Light Detection in Solar‐Blind Ultraviolet Region

“…[10][11][12] This structural feature can induce chirality into inorganic sublattice band edge states, allowing efficient charge transport and at the same time, chiroptical activity of these hybrid materials. [13][14][15][16][17] So far, prominent CPL photodetectors based on chiral HOIPs have been achieved (e.g., [(R)-NEA]PbI 3 , [(R)-MPA] 2 MAPb 2 I 7 , [(R)-/(S)-MBA]PbI 4 , and [(R)-/(S)-PEA]PbI 3 ), fully revealing their promise in this field. [18][19][20][21][22] Despite such an advance, however, those presented devices are characterized only at wavelengths in visible bands and typically achieve anisotropy factor of less than 0.2.…”