Ultrafast Control of Excitonic Rashba Fine Structure by Phonon Coherence in the Metal Halide Perovskite 
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Liu, Zhaoyu; Vaswani, Chirag; Yang, Xu; Zhao, Xin; Yao, Yongxin; Song, Zhaoning; Cheng, Di; Shi, Yongliang; Luo, Liang; Mudiyanselage, Dinusha Herath; Huang, Chih‐Ting; Park, Joong-Mok; Kim, Richard H. J.; Zhao, Jinping; Yan, Yuli; Ho, Kai‐Ming; Wang, Jigang

doi:10.1103/physrevlett.124.157401

Cited by 39 publications

(22 citation statements)

References 37 publications

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“…We characterize the THz quantum quench coherent dynamics directly in the time domain [31][32][33] (Methods) by measuring the responses to two phase-locked THz pulses as differential field transmission of the weak THz probe field ΔE/E 0 (blue circles, Fig. 1d) for THz pump field, E pump = 56 kV/cm and as a function of pump-probe time delay Δt pp .…”

Section: Resultsmentioning

confidence: 99%

Light quantum control of persisting Higgs modes in iron-based superconductors

et al. 2021

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The Higgs mechanism, i.e., spontaneous symmetry breaking of the quantum vacuum, is a cross-disciplinary principle, universal for understanding dark energy, antimatter and quantum materials, from superconductivity to magnetism. Unlike one-band superconductors (SCs), a conceptually distinct Higgs amplitude mode can arise in multi-band, unconventional superconductors via strong interband Coulomb interaction, but is yet to be accessed. Here we discover such hybrid Higgs mode and demonstrate its quantum control by light in iron-based high-temperature SCs. Using terahertz (THz) two-pulse coherent spectroscopy, we observe a tunable amplitude mode coherent oscillation of the complex order parameter from coupled lower and upper bands. The nonlinear dependence of the hybrid Higgs mode on the THz driving fields is distinct from any known SC results: we observe a large reversible modulation of resonance strength, yet with a persisting mode frequency. Together with quantum kinetic modeling of a hybrid Higgs mechanism, distinct from charge-density fluctuations and without invoking phonons or disorder, our result provides compelling evidence for a light-controlled coupling between the electron and hole amplitude modes assisted by strong interband quantum entanglement. Such light-control of Higgs hybridization can be extended to probe many-body entanglement and hidden symmetries in other complex systems.

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Section: Resultsmentioning

confidence: 99%

Light quantum control of persisting Higgs modes in iron-based superconductors

et al. 2021

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“…Deviations away from the perfect octahedral arrangement, even if only dynamic, i.e., upon excitation of an optical phonon, lift the degeneracy of the p-states and the inversion symmetry. [39] Lifting of the inversion symmetry leads to ferroelectric behavior. It is also one of the conditions to observe the Rashba effect.…”

Section: Discussionmentioning

confidence: 99%

Halide Perovskites: Advanced Photovoltaic Materials Empowered by a Unique Bonding Mechanism

Wuttig

Schön

Schumacher

et al. 2021

Adv Funct Materials

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Outstanding photovoltaic (PV) materials combine a set of advantageous properties including large optical absorption and high charge carrier mobility, facilitated by small effective masses. Halide perovskites (ABX 3 , where X = I, Br, or Cl) are among the most promising PV materials. Their optoelectronic properties are governed by the BX bond, which is responsible for the pronounced optical absorption and the small effective masses of the charge carriers. These properties are frequently attributed to the ns 2 configuration of the B atom, i.e., Pb 6s 2 or Sn 5s 2 ("lone-pair") states. The analysis of the PV properties in conjunction with a quantum-chemical bond analysis reveals a different scenario. The BX bond differs significantly from ionic, metallic, or conventional 2c2e covalent bonds. Instead it is better regarded as metavalent, since it shares about one p-electron between adjacent atoms. The resulting σ-bond, formally a 2c1e bond, is half-filled, causing pronounced optical absorption. Electron transfer between B and X atoms and lattice distortions open a moderate bandgap resulting in charge carriers with small effective masses. Hence, metavalent bonding explains favorable PV properties of halide perovskites, as summarized in a map for different bond types, which provides a blueprint to design PV materials.

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“…Lead-halide perovskite nanocrystals (NCs) have been heavily investigated for their intriguing properties, [1][2][3][4][5] including broad spectral tunability with anion [6][7][8] and cation [9][10][11][12][13] replacement, unique electronic structure, [14][15][16] and high defect tolerance. [17][18][19][20] These properties have made such NCs a popular emitter for application in light-emitting diodes (LEDs), [21][22] lasers, [23][24][25][26] single-photon sources, [27][28][29] and luminescent solar concentrators.…”

Section: Introductionmentioning

confidence: 99%

Modular Zwitterion-Functionalized Poly(Isopropyl Methacrylate) Polymers for Hosting Luminescent Lead-Halide Perovskite Nanocrystals

Cohen

Huang²,

Bricker³

et al. 2021

Preprint

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Inorganic lead-halide perovskite nanocrystals (NCs) are an exciting class of luminescent materials with high defect tolerance and broad spectral tunability, but such NCs are vulnerable to degradation under ambient conditions. Here, we report a class of modular zwitterion-functionalized isopropyl methacrylate polymers designed to stabilize a wide variety of perovskite NCs of different compositions, while also enabling processing in green solvents. Specifically, we report polymers in which the zwitterion spacing is tuned to accommodate the different lattice parameters of CsPb(Cl1-xBrx)3 and CsPbI3 NCs, and we report partially fluorinated polymers prepared to accommodate the needs of infrared-emitting NCs. We show that as-synthesized CsPbBr3, CsPbI3, and Yb3+:CsPbCl3 NCs are easily transferred into these zwitterionic polymers via a simple ligand-exchange procedure. These NC/polymer composites were then cast into thin films that showed substantially improved photoluminescence (PL) and stability compared with more conventional NC/polymer films. Specifically, CsPbBr3 and CsPbI3 NCs in films of their appropriately designed polymers had PL quantum yields of ~90% and ~80%, respectively. PL quantum yields decreased under continuous illumination, but self-healed completely after dark storage. We also found that all the NC compositions studied here maintain their PL quantum yields in NC/polymer composite films even after 1 year of ambient storage. These encouraging results demonstrate the utility of such modular zwitterion-functionalized polymers for hosting specific perovskite NCs, potentially opening avenues for robust new photonic applications of this important class of NCs.

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Ultrafast Control of Excitonic Rashba Fine Structure by Phonon Coherence in the Metal Halide Perovskite CH3NH3PbI3<

Cited by 39 publications

References 37 publications

Light quantum control of persisting Higgs modes in iron-based superconductors

Light quantum control of persisting Higgs modes in iron-based superconductors

Halide Perovskites: Advanced Photovoltaic Materials Empowered by a Unique Bonding Mechanism

Modular Zwitterion-Functionalized Poly(Isopropyl Methacrylate) Polymers for Hosting Luminescent Lead-Halide Perovskite Nanocrystals

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