Ultrafast quasiparticle dynamics in the correlated semimetal Ca3Ru2O7
Abstract
The correlated polar semimetal Ca3Ru2O7 exhibits a rich phase diagram including two magnetic transitions (TN = 56 K and TC = 48 K) with the appearance of an insulating-like pseudogap (at TC). In addition, there is a crossover back to metallic behavior at T* = 30 K, the origin of which is still under debate. We utilized ultrafast optical-pump optical-probe spectroscopy to investigate quasiparticle dynamics as a function of temperature in this enigmatic quantum material. We identify two dynamical processes, both of which are influenced by the onset of the pseudogap. This includes electron-phonon relaxation and, below TC, the onset of a phonon bottleneck hindering the relaxation of quasiparticles across the pseudogap. We introduce a gap-modified two-temperature model to describe the temperature dependence of electron-phonon thermalization, and use the Rothwarf-Taylor to model the phonon bottleneck. In conjunction with density functional theory, our experimental results synergistically reveal the origin of the T-dependent pseudogap. Further, our data and analysis indicate that T* emerges as a natural consequence of T-dependent gapping out of carriers, and does not correspond to a separate electronic transition. Furthermore, our results highlight the value of low-fluence ultrafast optics as a sensitive probe of low-energy electronic structure, thermodynamic parameters,more »
- Authors:
-
- Pennsylvania State University, University Park, PA (United States)
- University of California San Diego, La Jolla, CA (United States)
- Northwestern University, Evanston, IL (United States)
- Tulane University, New Orleans, LA (United States)
- Tulane University, New Orleans, LA (United States); Pennsylvania State University, University Park, PA (United States)
- Publication Date:
- Research Org.:
- Louisiana State Univ., Baton Rouge, LA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1611798
- Alternate Identifier(s):
- OSTI ID: 1505002; OSTI ID: 1670462
- Grant/Contract Number:
- SC0012432; SC00012375
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review B
- Additional Journal Information:
- Journal Volume: 99; Journal Issue: 15; Journal ID: ISSN 2469-9950
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; Materials Science; Physics; Density of states; Electrical conductivity; Fermi surface; First-principle calculations; Quasiparticles & collective excitations; Thermal properties; Single crystal materials; Strongly correlated systems; Ultrafast pump-probe spectroscopy
Citation Formats
Yuan, Yakun, Kissin, Peter, Puggioni, Danilo, Cremin, Kevin, Lei, Shiming, Wang, Yu, Mao, Zhiqiang, Rondinelli, James M., Averitt, Richard D., and Gopalan, Venkatraman. Ultrafast quasiparticle dynamics in the correlated semimetal Ca3Ru2O7. United States: N. p., 2019.
Web. doi:10.1103/physrevb.99.155111.
Yuan, Yakun, Kissin, Peter, Puggioni, Danilo, Cremin, Kevin, Lei, Shiming, Wang, Yu, Mao, Zhiqiang, Rondinelli, James M., Averitt, Richard D., & Gopalan, Venkatraman. Ultrafast quasiparticle dynamics in the correlated semimetal Ca3Ru2O7. United States. https://doi.org/10.1103/physrevb.99.155111
Yuan, Yakun, Kissin, Peter, Puggioni, Danilo, Cremin, Kevin, Lei, Shiming, Wang, Yu, Mao, Zhiqiang, Rondinelli, James M., Averitt, Richard D., and Gopalan, Venkatraman. Thu .
"Ultrafast quasiparticle dynamics in the correlated semimetal Ca3Ru2O7". United States. https://doi.org/10.1103/physrevb.99.155111. https://www.osti.gov/servlets/purl/1611798.
@article{osti_1611798,
title = {Ultrafast quasiparticle dynamics in the correlated semimetal Ca3Ru2O7},
author = {Yuan, Yakun and Kissin, Peter and Puggioni, Danilo and Cremin, Kevin and Lei, Shiming and Wang, Yu and Mao, Zhiqiang and Rondinelli, James M. and Averitt, Richard D. and Gopalan, Venkatraman},
abstractNote = {The correlated polar semimetal Ca3Ru2O7 exhibits a rich phase diagram including two magnetic transitions (TN = 56 K and TC = 48 K) with the appearance of an insulating-like pseudogap (at TC). In addition, there is a crossover back to metallic behavior at T* = 30 K, the origin of which is still under debate. We utilized ultrafast optical-pump optical-probe spectroscopy to investigate quasiparticle dynamics as a function of temperature in this enigmatic quantum material. We identify two dynamical processes, both of which are influenced by the onset of the pseudogap. This includes electron-phonon relaxation and, below TC, the onset of a phonon bottleneck hindering the relaxation of quasiparticles across the pseudogap. We introduce a gap-modified two-temperature model to describe the temperature dependence of electron-phonon thermalization, and use the Rothwarf-Taylor to model the phonon bottleneck. In conjunction with density functional theory, our experimental results synergistically reveal the origin of the T-dependent pseudogap. Further, our data and analysis indicate that T* emerges as a natural consequence of T-dependent gapping out of carriers, and does not correspond to a separate electronic transition. Furthermore, our results highlight the value of low-fluence ultrafast optics as a sensitive probe of low-energy electronic structure, thermodynamic parameters, and transport properties of Ruddlesden-Popper ruthenates.},
doi = {10.1103/physrevb.99.155111},
journal = {Physical Review B},
number = 15,
volume = 99,
place = {United States},
year = {Thu Apr 04 00:00:00 EDT 2019},
month = {Thu Apr 04 00:00:00 EDT 2019}
}
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Cited by: 7 works
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Figures / Tables:
Figure 1: (a) Atomic structure of Ca3Ru2O7 with a Bb21m space group. Ca, Ru, and O atoms are labeled in blue, brown and red, respectively. (b) DC resistivity of Ca3Ru2O7 in the a-b plane. Regions with different colors represent different behaviors emerging at low temperature. PM stands for paramagnetic phase.more »
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