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S. P. Moeller

Publications and source records attributed to S. P. Moeller.

3 recordsLinked to original sources

Persistent short-range charge correlations revealed by ultrafast melting of electronic order in YBa$_2$Cu$_3$O$_{6+x}$

Charge density waves (CDW) are ubiquitous in the complex phase diagram of cuprate superconductors and exhibit both short- and long-range correlations. Using time-resolved resonant X-ray scattering, we investigate the photo-induced dynamics of CDW in YBa$_2$Cu$_3$O$_{6.67}$. We discover an excitation threshold ($Φ$$_\mathrm{C}$ $\approx$ 65 $μ$J/cm$^2$) above which long-range CDW disappear, revealing a persistent CDW peak with short-range correlation length. Ultrafast photo-excitation promptly uncovers this residual short-range CDW correlations, appearing within $\approx$ 0.2 ps. Long-range CDW coherence recovers within $\approx$ 0.6 ps, while the peak intensity remains partially suppressed. We rationalize the dichotomic behavior in the fluence and temporal dependencies as the signature of two coexisting CDW peaks, arising from short- and long-range correlations, which we disentangle through their distinct response to photo-excitation. We provide evidence that the collapse of long-range correlations is driven by an electronic process, while short-range correlations are characterized by distinct timescales and stiffness against photo-excitation. This approach establishes ultrafast X-ray scattering as an effective tool for disentangling coexisting density waves and correlations in quantum materials.

cond-mat.supr-con

Enhanced charge density wave coherence in a light-quenched, high-temperature superconductor

Superconductivity and charge density waves (CDW) are competitive, yet coexisting orders in cuprate superconductors. To understand their microscopic interdependence, a probe capable of discerning their interaction on its natural length and time scales is necessary. We use ultrafast resonant soft x-ray scattering to track the transient evolution of CDW correlations in YBa$_{2}$Cu$_{3}$O$_{6+x}$ following the quench of superconductivity by an infrared laser pulse. We observe a non-thermal response of the CDW order characterized by a near doubling of the correlation length within $\approx$ 1 picosecond of the superconducting quench. Our results are consistent with a model in which the interaction between superconductivity and CDW manifests inhomogeneously through disruption of spatial coherence, with superconductivity playing the dominant role in stabilizing CDW topological defects, such as discommensurations.

cond-mat.supr-con

Probing ultrafast ππ*/nπ* internal conversion in organic chromophores via K-edge resonant absorption

Organic chromophores with heteroatoms possess an important excited state relaxation channel from an optically allowed ππ* to a dark nπ*state. We exploit the element and site specificity of soft x-ray absorption spectroscopy to selectively follow the electronic change during the ππ*/nπ* internal conversion. As a hole forms in the n orbital during ππ*/nπ* internal conversion, the near edge x-ray absorption fine structure (NEXAFS) spectrum at the heteroatom K-edge exhibits an additional resonance. We demonstrate the concept with the nucleobase thymine, a prototypical heteroatomic chromophore. With the help of time resolved NEXAFS spectroscopy at the oxygen K-edge, we unambiguously show that ππ*/nπ* internal conversion takes place within (60 \pm 30) fs. High-level coupled cluster calculations on the isolated molecules used in the experiment confirm the superb electronic structure sensitivity of this new method for excited state investigations.

physics.chem-ph