How Exciton Interactions Control Spin-Depolarization in Layered Hybrid Perovskites

被引：36

作者：

Bourelle, Sean A. ^{[1
]}

Shivanna, Ravichandran ^{[1
]}

Camargo, Franco V. A. ^{[2
]}

Ghosh, Soumen ^{[2
]}

Gillett, Alexander J. ^{[1
]}

Senanayak, Satyaprasad P. ^{[1
,3
]}

Feldmann, Sascha ^{[1
]}

Eyre, Lissa ^{[1
,4
]}

Ashoka, Arjun ^{[1
]}

van de Goor, Tim W. J. ^{[1
]}

Abolins, Haralds ^{[1
]}

Winkler, Thomas ^{[1
]}

Cerullo, Giulio ^{[2
]}

Friend, Richard H. ^{[1
]}

Deschler, Felix ^{[4
]}

机构：

[1] Univ Cambridge, Cavendish Lab, Cambridge CB3 0HE, England

[2] Politecn Milan, Dipartimento Fis, IFN CNR, I-20133 Milan, Italy

[3] CSIR Inst Minerals & Mat Technol, Bhubaneswar 751013, India

[4] Tech Univ Munich, Walter Schottky Inst, Phys Dept, D-85748 Garching, Germany

来源：

NANO LETTERS | 2020年 / 20卷 / 08期

基金：

英国工程与自然科学研究理事会; 欧盟地平线“2020”;

关键词：

2D perovskites; many body interactions; spin; exciton; total angular momentum; transient absorption spectroscopy; LEAD IODIDE PEROVSKITE; SINGLE-CRYSTAL; FREE-CARRIERS; DYNAMICS; RELAXATION; EFFICIENCY;

D O I：

10.1021/acs.nanolett.0c00867

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

Using circularly polarized broadband transient absorption, time-resolved circular photoluminescence, and transient Faraday rotation spectroscopy, we report that spin-dependent interactions have a significant impact on exciton energies and spin depolarization times in layered Ruddlesden-Popper hybrid metal-halide perovskites. In BA(2)FAPb(2)I(7), we report that room-temperature spin lifetimes are largest (3.2 ps) at a carrier density of similar to 10(17) cm(-3) with increasing depolarization rates at higher exciton densities. This indicates that many-body interactions reduce spin-lifetimes and outcompete the effect of D'yakonov-Perel precessional relaxation that has been previously reported at lower carrier densities. We further observe a dynamic circular dichroism that arises from a photoinduced polarization in the exciton distribution between total angular momentum states. Our findings provide fundamental and application relevant insights into the spin-dependent exciton-exciton interactions in layered hybrid perovskites.

引用

页码：5678 / 5685

页数：8

共 55 条

[1] Exciton-polariton spin switches [J].

Amo, A. ;

Liew, T. C. H. ;

Adrados, C. ;

Houdre, R. ;

Giacobino, E. ;

Kavokin, A. V. ;

Bramati, A. .

NATURE PHOTONICS, 2010, 4 (06) :361-366

[2] Bright triplet excitons in caesium lead halide perovskites [J].

Becker, Michael A. ;

Vaxenburg, Roman ;

Nedelcu, Georgian ;

Sercel, Peter C. ;

Shabaev, Andrew ;

Mehl, Michael J. ;

Michopoulos, John G. ;

Lambrakos, Samuel G. ;

Bernstein, Noam ;

Lyons, John L. ;

Stoferle, Thilo ;

Mahrt, Rainer F. ;

Kovalenko, Maksym V. ;

Norris, David J. ;

Raino, Gabriele ;

Efros, Alexander L. .

NATURE, 2018, 553 (7687) :189-+

[3] Coherent spin dynamics of electrons and holes in CsPbBr3 perovskite crystals [J].

Belykh, Vasilii V. ;

Yakovlev, Dmitri R. ;

Glazov, Mikhail M. ;

Grigoryev, Philipp S. ;

Hussain, Mujtaba ;

Rautert, Janina ;

Dirin, Dmitry N. ;

Kovalenko, Maksym V. ;

Bayer, Manfred .

NATURE COMMUNICATIONS, 2019, 10 (1)

[4] Impact of Layer Thickness on the Charge Carrier and Spin Coherence Lifetime in Two-Dimensional Layered Perovskite Single Crystals [J].

Chen, Xihan ;

Lu, Haipeng ;

Li, Zhen ;

Zhai, Yaxin ;

Ndione, Paul F. ;

Berry, Joseph J. ;

Zhu, Kai ;

Yang, Ye ;

Beard, Matthew C. .

ACS ENERGY LETTERS, 2018, 3 (09) :2273-2279

[5] Radiative recombination processes in wide-band-gap II-VI quantum wells: The interplay between excitons and free carriers [J].

Cingolani, R ;

Calcagnile, L ;

Coli, G ;

Rinaldi, R ;

Lomoscolo, M ;

DiDio, M ;

Franciosi, A ;

Vanzetti, L ;

LaRocca, GC .

JOURNAL OF THE OPTICAL SOCIETY OF AMERICA B-OPTICAL PHYSICS, 1996, 13 (06) :1268-1277

[6] Mixture of composite-boson molecules and the Pauli exclusion principle [J].

Combescot, M. ;

Betbeder-Matibet, O. ;

Dubin, F. .

PHYSICAL REVIEW A, 2007, 76 (03)

[7] Time evolution of two ground-state excitons [J].

Combescot, M. ;

Betbeder-Matibet, O. .

PHYSICAL REVIEW B, 2010, 81 (23)

[8] The inconstant world of composite excitons [J].

Combescot, Monique .

SUPERLATTICES AND MICROSTRUCTURES, 2008, 43 (5-6) :394-398

[9] The many-body physics of composite bosons [J].

Combescot, Monique ;

Betbeder-Matibet, Odile ;

Dubin, Francois .

PHYSICS REPORTS-REVIEW SECTION OF PHYSICS LETTERS, 2008, 463 (5-6) :215-318

[10] Optical spin resonance and transverse spin relaxation in magnetic semiconductor quantum wells [J].

Crooker, SA ;

Awschalom, DD ;

Baumberg, JJ ;

Flack, F ;

Samarth, N .

PHYSICAL REVIEW B, 1997, 56 (12) :7574-7588

← 1 2 3 4 5 6 →