Transient and steady state magneto-optical studies of the 
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 crystal

Huynh, Uyen; Feng, Teddy; Khanal, Dipak Raj; Liu, Hui; Bailey, Paul; Bodin, Rikard; Sercel, Peter C.; Huang, Jinsong; Vardeny, Z. Valy

doi:10.1103/physrevb.106.094306

Cited by 5 publications

(5 citation statements)

References 31 publications

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“…The intrinsic exciton Landé g int factor is estimated as 0.67. Our measured exciton g int factor is significantly smaller than literature reports of halide perovskites, which are generally in the range of 2.1–2.7 . This difference may be attributed to the much smaller magnetic fields (1.6 T) used in our MCD measurements, whereas literature reports generally use over 15 T magnetic fields.…”

Section: Resultscontrasting

confidence: 76%

“…Our measured exciton g int factor is significantly smaller than literature reports of halide perovskites, which are generally in the range of 2.1−2.7. 33 This difference may be attributed to the much smaller magnetic fields (1.6 T) used in our MCD measurements, whereas literature reports generally use over 15 T magnetic fields. For Mn 2+ -doped chiral perovskites, a second term arises from Mn 2+ ions due to the sp−d interactions,…”

Section: Resultsmentioning

confidence: 85%

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Induced Circularly Polarized Luminescence and Exciton Fine Structure Splitting in Magnetic-Doped Chiral Perovskites

Zhang,

Liang,

Xue

et al. 2024

ACS Nano

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Magnetic impurity doping in semiconductors has emerged as an important strategy to endow exotic photophysical and magnetic properties. While most reported hosts are centrosymmetric semiconductors, doping magnetic ions into a noncentrosymmetric chiral semiconductor can offer additional control of photonic and spin polarization. In this work, we synthesized a Mn 2+ -doped chiral two-dimensional (2D) perovskite, Mn 2+ :(R-MPA) 2 PbBr 4 (R-MPA + = R-methyl phenethylammonium). We found that the optical activity of chiral 2D perovskites is enhanced with an increased concentration of Mn 2+ ions. Additionally, efficient energy transfer from the chiral host to the Mn 2+ dopants is observed. This energy transfer process gives rise to circularly polarized luminescence from the excited state of Mn 2+ ( 4 T 1 → 6 A 1 ), exhibiting a photoluminescence quantum yield up to 24% and a dissymmetry factor of 11%. The exciton fine structures of undoped and Mn 2+ -doped (R-MPA) 2 PbBr 4 are further studied through magnetic circular dichroism (MCD) spectroscopy. Our analysis shows that chiral organic cations lead to an exciton fine structure splitting energy as large as 5.0 meV, and the splitting is further increased upon Mn 2+ doping. Our results reveal the strong impacts of molecular chirality and magnetic dopants on the exciton structures of halide perovskites.

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Section: Resultscontrasting

confidence: 76%

Section: Resultsmentioning

confidence: 85%

Induced Circularly Polarized Luminescence and Exciton Fine Structure Splitting in Magnetic-Doped Chiral Perovskites

Zhang,

Liang,

Xue

et al. 2024

ACS Nano

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“…For measuring the spin lifetime in CsPbBr 3 single crystals, we have used the ultrafast circularly-polarized photoinduced reflectivity (PPR) method at liquid He temperature under the influence of a magnetic field. The experimental setup was described elsewhere 10 , 63 . It is a derivative of the well-known ‘pump-probe’ technique, where the polarization of the pump beam is modulated by a photoelastic modulator between left ( δ + ) and right ( δ − ) circular polarization, namely LCP and RCP, respectively.…”

Section: Methodsmentioning

confidence: 99%

“…The pump/probe beams having average intensity of 12 Wcm −2 and 3 Wcm −2 , respectively were aligned onto the CsPbBr 3 crystal that was placed inside a cryostat with a built-in electro-magnet that delivered a field strength, B up to 700 mT at temperatures down to 4 K. Using this technique we measured both t-PPR responses at both zero and finite B to extract the B -dependent electron and hole spin lifetimes. From the c-PPR( B , t ) dynamics measured on (001) facet with B directed along [010] 63 (see example c-PPR( B , t ) dynamics in SI Fig. S15) , we could obtain the electron and hole by fitting the transient quantum beating response with two damped oscillation functions: where and are the spin dephasing times of the electrons and holes; f1 and f2 are the two QB frequencies that can be obtained directly from the fast Fourier transform of the c-PPR dynamics.…”

Section: Methodsmentioning

confidence: 99%

How spin relaxes and dephases in bulk halide perovskites

Xu,

Li,

Huynh

et al. 2024

Nat Commun

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Spintronics in halide perovskites has drawn significant attention in recent years, due to their highly tunable spin-orbit fields and intriguing interplay with lattice symmetry. Here, we perform first-principles calculations to determine the spin relaxation time (T1) and ensemble spin dephasing time ($${T}_{2}^{*}$$ T 2 * ) in a prototype halide perovskite, CsPbBr3. To accurately capture spin dephasing in external magnetic fields we determine the Landé g-factor from first principles and take it into account in our calculations. These allow us to predict intrinsic spin lifetimes as an upper bound for experiments, identify the dominant spin relaxation pathways, and evaluate the dependence on temperature, external fields, carrier density, and impurities. We find that the Fröhlich interaction that dominates carrier relaxation contributes negligibly to spin relaxation, consistent with the spin-conserving nature of this interaction. Our theoretical approach may lead to new strategies to optimize spin and carrier transport properties.

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“…One has to keep in mind that the effective nuclear field experienced by the carriers should be multiplied by the carrier g-factor in order to obtain values that can be compared to each other. Despite the general trend of [9] 32−53 5.2 1.9 30 14 CsPbBr 3 [38] 5.6 2 polycrystalline films MAPbI 3 film [39,40] 4.4 7 MAPb(Cl,I) 3 film [8] 0.8 0.2 CsPbBr 3 film [41] 0.05 0. the importance of the nuclear fluctuations on the spin dynamics, a quantitative evaluation for several materials cannot be drawn yet. Interestingly, the activation energies of FAPbBr 3 are somewhat closer to those of other hybrid organic−inorganic perovskites than to those in all-inorganic perovskites.…”

mentioning

confidence: 98%

Coherent Carrier Spin Dynamics in FAPbBr₃Perovskite Crystals

Kirstein,

Zhukov,

Yakovlev

et al. 2024

J. Phys. Chem. Lett.

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Coherent spin dynamics of electrons and holes are studied in hybrid organic− inorganic lead halide perovskite FAPbBr 3 bulk single crystals using the time-resolved Kerr ellipticity technique at cryogenic temperatures. The Larmor spin precession of the carrier spins in a magnetic field is monitored to measure the Landég-factors of electrons (+2.44) and holes (+0.41). These g-factors are highly isotropic. The measured spin dephasing times amount to a few nanoseconds, and the longitudinal hole spin relaxation time is 470 ns. The important role of the strong hyperfine interaction between carrier spins and nuclear spins is demonstrated via dynamic nuclear polarization. At low temperatures, electron and hole spin relaxation predominantly occurs via the hyperfine interaction, whose importance significantly decreases at temperatures above 12 K. We overview the spin dynamics in various lead halide perovskite crystals and polycrystalline films and conclude on their common features provided by charge carrier localization at cryogenic temperatures.

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Transient and steady state magneto-optical studies of the CsPbBr3 crystal

Cited by 5 publications

References 31 publications

Induced Circularly Polarized Luminescence and Exciton Fine Structure Splitting in Magnetic-Doped Chiral Perovskites

Induced Circularly Polarized Luminescence and Exciton Fine Structure Splitting in Magnetic-Doped Chiral Perovskites

How spin relaxes and dephases in bulk halide perovskites

Coherent Carrier Spin Dynamics in FAPbBr₃Perovskite Crystals

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Transient and steady state magneto-optical studies of the CsPbBr3 crystal

Cited by 5 publications

References 31 publications

Induced Circularly Polarized Luminescence and Exciton Fine Structure Splitting in Magnetic-Doped Chiral Perovskites

Induced Circularly Polarized Luminescence and Exciton Fine Structure Splitting in Magnetic-Doped Chiral Perovskites

How spin relaxes and dephases in bulk halide perovskites

Coherent Carrier Spin Dynamics in FAPbBr3Perovskite Crystals

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Product

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Coherent Carrier Spin Dynamics in FAPbBr₃Perovskite Crystals