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Multi-mode excitation drives disorder during the ultrafast melting of a C4-symmetry-broken phase.

ABSTRACT: Spontaneous C₄-symmetry breaking phases are ubiquitous in layered quantum materials, and often compete with other phases such as superconductivity. Preferential suppression of the symmetry broken phases by light has been used to explain non-equilibrium light induced superconductivity, metallicity, and the creation of metastable states. Key to understanding how these phases emerge is understanding how C₄ symmetry is restored. A leading approach is based on time-dependent Ginzburg-Landau theory, which explains the coherence response seen in many systems. However, we show that, for the case of the single layered manganite La_0.5Sr_1.5MnO_4, the theory fails. Instead, we find an ultrafast inhomogeneous disordering transition in which the mean-field order parameter no longer reflects the atomic-scale state of the system. Our results suggest that disorder may be common to light-induced phase transitions, and methods beyond the mean-field are necessary for understanding and manipulating photoinduced phases.

SUBMITTER: Perez-Salinas D

PROVIDER: S-EPMC8752725 | biostudies-literature | 2022 Jan

REPOSITORIES: biostudies-literature

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Multi-mode excitation drives disorder during the ultrafast melting of a C4-symmetry-broken phase.

Perez-Salinas Daniel D Johnson Allan S AS Prabhakaran Dharmalingam D Wall Simon S

Nature communications 20220111 1

Spontaneous C<sub>4</sub>-symmetry breaking phases are ubiquitous in layered quantum materials, and often compete with other phases such as superconductivity. Preferential suppression of the symmetry broken phases by light has been used to explain non-equilibrium light induced superconductivity, metallicity, and the creation of metastable states. Key to understanding how these phases emerge is understanding how C<sub>4</sub> symmetry is restored. A leading approach is based on time-dependent Gin ...[more]

PMID: 35017507

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Project description:Achieving long-lived symmetry-broken charge-separated states in chromophoric assemblies is quintessential for enhanced performance of artificial photosynthetic mimics. However, the occurrence of energy trap states hinders exciton and charge transport across photovoltaic devices, diminishing power conversion efficiency. Herein, we demonstrate unprecedented excimer formation in the relaxed excited-state geometry of bichromophoric systems impeding the lifetime of symmetry-broken charge-separated states. Core-annulated perylenediimide dimers (SC-SPDI2 and SC-NPDI2) prefer a near-orthogonal arrangement in the ground state and a π-stacked foldamer structure in the excited state. The prospect of an excimer-like state in the foldameric arrangement of SC-SPDI2 and SC-NPDI2 has been rationalized by fragment-based excited state analysis and temperature-dependent photoluminescence measurements. Effective electronic coupling matrix elements in the Franck-Condon geometry of SC-SPDI2 and SC-NPDI2 facilitate solvation-assisted ultrafast symmetry-breaking charge-separation (SB-CS) in a high dielectric environment, in contrast to unrelaxed excimer formation (Ex*) in a low dielectric environment. Subsequently, the SB-CS state dissociates into an undesired relaxed excimer state (Ex) due to configuration mixing of a Frenkel exciton (FE) and charge-separated state in the foldamer structure, downgrading the efficacy of the charge-separated state. The decay rate constant of the FE to SB-CS (k FE→SB-CS) in polar solvents is 8-17 fold faster than that of direct Ex* formation (k FE→Ex*) in non-polar solvent (k FE→SB-CS≫k FE→Ex*), characterized by femtosecond transient absorption (fsTA) spectroscopy. The present investigation establishes the impact of detrimental excimer formation on the persistence of the SB-CS state in chromophoric dimers and offers the requisite of conformational rigidity as one of the potential design principles for developing advanced molecular photovoltaics.

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Multi-mode excitation drives disorder during the ultrafast melting of a C4-symmetry-broken phase.

Publications

Multi-mode excitation drives disorder during the ultrafast melting of a C4-symmetry-broken phase.

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