Ultrafast zero-bias photocurrent and terahertz emission in hybrid perovskites

Obraztsov, Petr A.; Lyashenko, D. A.; Chizhov, P. A.; Konishi, Kuniaki; Nemoto, Natsuki; Kuwata‐Gonokami, Makoto; Welch, Eric; Obraztsov, A. N.; Zakhidov, Alex

doi:10.1038/s42005-018-0013-8

Cited by 35 publications

(45 citation statements)

References 39 publications

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“…Furthermore, the sense of spin is opposite at the valley and peak of the CPGE-EX spectrum. We thus conclude that the spin-dependent photocurrent associated with the photogenerated excitons is a feature that cannot be explained by the CPGE traditional band model 30,35,36 .…”

Section: Resultsmentioning

confidence: 76%

“…Therefore, there is associated terahertz (THz) radiation from the resulting time-varying current 35 . At steady state conditions, the continuous generation of spin-polarized free carriers leads to a continuous-wave (cw) photocurrent that is sensitive to the polarization status of excitation light 30,35,36 . Since the group velocity of free carriers at the bottom (top) of CB (VB) is zero ( Fig.…”

Section: Resultsmentioning

confidence: 99%

“…1c. The 4α terms describe LPGE, the 2α terms stand for CPGE, and D represents a polarization-independent offset that originates from other effects such as photothermal, photovoltaic response, or photo-Dember effect 30,35,36,40 . The cosine term, C2 is mainly due to misalignment (about 1~3 degree, in our case) between the fast axis of the λ/4 waveplate and the incident light polarization, so that C2«C1.…”

Section: Resultsmentioning

confidence: 99%

“…CPGE has been studied in a variety of Rashba type materials including doped GaAs/AlGaAs MQW 31 , the polar semiconductor BiTeI 32 , 2D transition-metal dichalcogenides 33 , and topological insulator 34 . Most recently, the CPGE was studied in bulk methylammonium lead iodide perovskite (MAPbI 3 ) films 35 and single crystal 36 . Here we employ helicity-dependent steady state layers, which form natural multiple quantum wells (MQW), where the inorganic layer is the potential 'well' and organic layer is the potential 'wall'.…”

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confidence: 99%

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Circular photogalvanic spectroscopy of Rashba splitting in 2D hybrid organic–inorganic perovskite multiple quantum wells

et al. 2020

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The two-dimensional (2D) Ruddlesden−Popper organic-inorganic halide perovskites such as (2D)-phenethylammonium lead iodide (2D-PEPI) have layered structure that resembles multiple quantum wells (MQW). The heavy atoms in 2D-PEPI contribute a large spin-orbit coupling that influences the electronic band structure. Upon breaking the inversion symmetry, a spin splitting ('Rashba splitting') occurs in the electronic bands. We have studied the spin splitting in 2D-PEPI single crystals using the circular photogalvanic effect (CPGE). We confirm the existence of Rashba splitting at the electronic band extrema of 35±10 meV, and identify the main inversion symmetry breaking direction perpendicular to the MQW planes. The CPGE action spectrum above the bandgap reveals spin-polarized photocurrent generated by ultrafast relaxation of excited photocarriers separated in momentum space. Whereas the helicity dependent photocurrent with below-gap excitation is due to spin-galvanic effect of the ionized spin-polarized excitons, where spin polarization occurs in the spin-split bands due to asymmetric spin-flip.

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Section: Resultsmentioning

confidence: 76%

Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

mentioning

confidence: 99%

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Circular photogalvanic spectroscopy of Rashba splitting in 2D hybrid organic–inorganic perovskite multiple quantum wells

et al. 2020

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“…Particularly, the shift current is expected to be important in hybrid organic–inorganic halide perovskites solar cells for their excellent PCE and achievable inversion symmetry broken by dipolar cation . Obraztsov et al has also measured the ultrafast photocurrent generation from CH 3 NH 3 PbI 3 and proved the BPVE due to the shift current …”

Section: Introductionmentioning

confidence: 99%

High‐Order Shift Current Induced Terahertz Emission from Inorganic Cesium Bromine Lead Perovskite Engendered by Two‐Photon Absorption

Huang

et al. 2019

Adv Funct Materials

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High-order nonlinear optical phenomena are interesting from a fundamental point of view as they reveal intrinsic symmetries of the materials. Potentially they can also be used for practical optoelectronic applications. High-order shift current is one of these phenomena, and yet it has never been detected in experiments, primarily due to the difficulty in conventional contact detection. In this work, the shift current due to the two-photon absorption (TPA) from all-inorganic perovskite CsPbBr 3 is first observed by a contactless and nondestructive terahertz (THz) emission method. The results reveal that the THz emission is dominated by a high-order shift current (fourth-order nonlinear optical effect) with the below-bandgap photon energy of femtosecond laser excitation. The high-order shift current origins from the broken inversion symmetry induced by the dynamic stereochemical activity of the Pb 2+ lone pair. A microscopic TPA-assisted nonlinear optical model is presented to describe the photophysical process of the THz emission. The model matches well with the quadratic pump fluence and angular dependence of the THz emission. This work can not only open a new venue for the all-inorganic perovskite-based nonlinear optoelectronics and THz devices, but also afford a THz technology for the high-order nonlinear effect analysis.

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

et al. 2021

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The circular photogalvanic effect (CPGE) is a novel spin-related optoelectronic phenomenon based on the SOC of noncentrosymmetric systems. [15] Under the CPGE, a steady photocurrent is generated by the irradiation of circularly polarized light (CPL) without an external bias voltage, and the photocurrent direction is reversed by switching the photon helicity. [15,16] The CPGE originates from the asymmetric distribution of photocarriers in a momentum space (k-space) excited by CPL in interband transitions with a spin-flip between the spin-splitting states (Scheme 1). [16] The direction of the zero-bias photocurrent can be controlled based on the helicity of the CPL, as the asymmetric distribution of photocarriers arises from the selection rule of CPL excitation, Δm J = ±1, where m J is the magnetic quantum number of the total angular momentum (Scheme 1). [16] Hence, noncentrosymmetric systems, wherein SOC could induce spin-splitting in electronic states, are promising platforms to generate the CPGE. In fact, the CPGE has been observed in various polar systems, such as group III-V compound semiconductors, [16][17][18][19] the surface of topological insulators, [20][21][22] a bulk Rashba semiconductor, [23] and transition metal dichalcogenides. [24][25][26][27] In these studies, the correlation between polarity and the CPGE was investigated in detail, andThe control of the optoelectronic properties of 2D organic-inorganic hybrid perovskite (2D-OIHP) lead halides is an increasingly prevalent topic. Herein, the observation of the circular photogalvanic effect (CPGE) in new enantiomorphic 2D-OIHP lead iodides is reported, which are synthesized as a first OIHP-related system belonging to a chiral space group by incorporating organic chiral cations into the inorganic layers of lead iodides. The CPGE is an optoelectronic phenomenon associated with the spin-orbit coupling of heavy atoms in noncentrosymmetric systems. Owing to the CPGE, lighthelicity-dependent steady photocurrents are generated without an external bias voltage under the irradiation of circularly polarized light. Furthermore, the sign reversal of the CPGE photocurrent depending on the chirality of the designed 2D-OIHP lead iodides is observed. This result indicates formation of the theoretically predicted radial spin-polarized texture in k-space of chiral systems owing to spin-momentum locking. Hence, chiral 2D-OIHP lead halides can be a promising platform for engineering opto-spintronic functionalities.

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Ultrafast zero-bias photocurrent and terahertz emission in hybrid perovskites

Abstract: On a macroscopic level both injection (CPGE) and shift (LPGE) currents can be linked to secondorder optical nonlinear effects, as

Cited by 35 publications

References 39 publications

Circular photogalvanic spectroscopy of Rashba splitting in 2D hybrid organic–inorganic perovskite multiple quantum wells

Circular photogalvanic spectroscopy of Rashba splitting in 2D hybrid organic–inorganic perovskite multiple quantum wells

High‐Order Shift Current Induced Terahertz Emission from Inorganic Cesium Bromine Lead Perovskite Engendered by Two‐Photon Absorption

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

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