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arXiv:1809.09204 · Physical review. B./Physical review. B

Efficient prediction of time- and angle-resolved photoemission spectroscopy measurements on a nonequilibrium BCS superconductor

Tianrui Xu, Takahiro Morimoto, Alessandra Lanzara, Joel E. Moore

Published Jan 9, 2019• 9 citations
arXivHTMLPDF

Abstract

We study how time- and angle-resolved photoemission (tr-ARPES) reveals the dynamics of BCS-type, $s$-wave superconducting systems with time-varying order parameters. Approximate methods are discussed, based on previous approaches to either optical conductivity or quantum dot transport, to enable computationally efficient prediction of photoemission spectra. One use of such predictions is to enable extraction of the underlying order parameter dynamics from experimental data, which is topical given the rapidly growing use of tr-ARPES in studying unconventional superconductivity. The methods considered model the two-time lesser Green's functions with an approximated lesser self-energy that describes relaxation by coupling of the system to two types of baths. The approach primarily used here also takes into consideration the relaxation of the excited states into equilibrium by explicitly including the level-broadening of the retarded and advanced Green's functions. We present equilibrium and nonequilibrium calculations of tr-ARPES spectrum from our model and discuss the signatures of different types of superconducting dynamics.

DOI
10.1103/physrevb.99.035117

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We study how time- and angle-resolved photoemission (tr-ARPES) reveals the dynamics of BCS-type, sss-wave superconducting systems with time-varying order parameters. Approximate methods are discussed, based on previous approaches to either optical conductivity or quantum dot transport, to enable computationally efficient prediction of photoemission spectra. One use of such predictions is to enable extraction of the underlying order parameter dynamics from experimental data, which is topical given the rapidly growing use of tr-ARPES in studying unconventional superconductivity. The methods considered model the two-time lesser Green's functions with an approximated lesser self-energy that describes relaxation by coupling of the system to two types of baths. The approach primarily used here also takes into consideration the relaxation of the excited states into equilibrium by explicitly including the level-broadening of the retarded and advanced Green's functions. We present equilibrium and nonequilibrium calculations of tr-ARPES spectrum from our model and discuss the signatures of different types of superconducting dynamics.
Higgs oscillations in nonequilibrium superconductors provide a unique tool to obtain information about the underlying order parameter. Several properties like the absolute value, existence of multiple gaps, and the symmetry of the order parameter can be encoded in the Higgs oscillation spectrum. Studying Higgs oscillations with time-resolved angle-resolved photoemission spectroscopy (ARPES) has the advantage over optical measurements that a momentum-resolved analysis of the condensate dynamic is possible. In this paper, we investigate the time-resolved spectral function measured in ARPES for different quench protocols. We find that analyzing amplitude oscillations of the ARPES intensity in the whole Brillouin zone allows to understand how the condensate dynamic contributes to the emerging of collective Higgs oscillations. Furthermore, by evaluating the phase of these oscillations, the symmetry deformation dynamic of the condensate can be revealed, which gives insight about the ground state symmetry of the system. With such an analysis, time-resolved ARPES experiments might be used in the future as a powerful tool in the field of Higgs spectroscopy.
The angle-resolved photoemission spectra (ARPES) of the spin-1/2 Holstein model at non-half-filling are calculated by using the adiabatic approximation and the classical Monte Carlo method. It is found that in the metallic state, the spectra take broad Gaussians at the band bottom, while evolving to sharp Lorentzians near the Fermi level, commonly in one, two, and three dimensions. We justify that this evolution in ARPES is connected with an electronic state transition from quasi-localized ones to the extended ones due to the scattering of electrons with the static lattice distortion.
Time-resolved photoemission experiments can reveal fascinating quantum dynamics of correlated electrons. However, the thermalization of the electronic system is typically so fast that very short probe pulses are necessary to resolve the time evolution of the quantum state, and this leads to poor energy resolution due to the energy-time uncertainty relation. Although the photoemission intensity can be calculated from the nonequilibrium electronic Green's functions, the converse procedure is therefore difficult. We analyze a hypothetical time-resolved photoemission experiment on a correlated electronic system, described by the Falicov-Kimball model in dynamical mean-field theory, which relaxes between metallic and insulating phases. We find that the real-time Green's function which describes the transient behavior during the buildup of the metallic state cannot be determined directly from the photoemission signal. On the other hand, the characteristic collapse-and-revival oscillations of an excited Mott insulator can be observed as oscillating weight in the center of the Mott gap in the time-dependent photoemission spectrum.
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We investigate radio-frequency (rf) spectroscopy, metal-to-superconductor tunneling, and angle-resolved photoemission spectroscopy (ARPES) as probes of isolated out-of-equilibrium quantum systems, and examine the crucial role played by the nonequilibrium distribution function. As an example, we focus on the induced topological time-periodic (Floquet) phase in a two-dimensional p+ipp+ipp+ip superfluid, following an instantaneous quench of the coupling strength. The post-quench Cooper pairs occupy a linear combination of ``ground'' and ``excited'' Floquet states, with coefficients determined by the distribution function. While the Floquet band structure exhibits a single avoided crossing relative to the equilibrium case, the distribution function shows a population inversion of the Floquet bands at low energies. For a realization in ultracold atoms, these two features compensate, producing a bulk average rf signal that is well captured by a quasiequilibrium approximation. In particular, the rf spectrum shows a robust gap. The single crossing occurs because the quench-induced Floquet phase belongs to a particular class of soliton dynamics for the BCS equation. The population inversion is a consequence of this, and ensures the conservation of the pseudospin winding number. As a comparison, we compute the rf signal when only the lower Floquet band is occupied; in this case, the gap disappears for strong quenches. The tunneling signal in a solid-state realization is ignorant of the distribution function, and can show wildly different behaviors. We also examine rf, tunneling, and ARPES for weak quenches, such that the resulting topological steady state is characterized by a constant nonequilibrium order parameter. In a system with a boundary, tunneling reveals the Majorana edge states. However, the local rf signal due to the edge states is suppressed by a factor of the inverse system size, and is spatially deconfined throughout the bulk of the sample.
Recent pump-probe experiments on underdoped cuprates and similar systems suggest the existence of a transient superconducting state above Tc{T}_{c}Tc​. This poses the question of how to reliably identify the emergence of long-range order, in particular superconductivity, out of equilibrium. We investigate this point by studying a quantum quench in an extended Hubbard model and by computing various observables, which are used to identify (quasi-)long-range order in equilibrium. Our findings imply that, in contrast to current experimental studies, it does not suffice to study the time evolution of the optical conductivity to identify superconductivity. In turn, we suggest to utilize time-resolved angle-resolved photoemission spectroscopy experiments to probe for the formation of a condensate in the two-particle channel.