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arXiv:1902.09549 · Physical review. B./Physical review. B

Higgs oscillations in time-resolved optical conductivity

Ankit Kumar, Alexander F. Kemper

Published Nov 21, 2019• 19 citations
arXivHTMLPDF

Abstract

Driving superconductors out of equilibrium is a promising avenue to study their equilibrium properties as well as to control the superconducting state. Nonequilibrium superconductors are often studied using time-resolved optical conductivity measurements. Thus, the characterization of a superconducting state in a pump driven nonequilibrium state requires careful attention in the time domain. We calculate the time-resolved optical conductivity of a pumped superconducting state using a nonequilibrium Keldysh approach. Through functional derivation, the optical conductivity is obtained with full vertex corrections and used to characterize the transient superconducting state. The transient optical conductivity shows the suppression of the superconducting order parameter in the time domain. The subsequent recovery of the order parameter exhibits oscillatory behavior that corresponds to the Higgs amplitude mode, and may be seen in several parts of the spectrum.

DOI
10.1103/physrevb.100.174515

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Driving superconductors out of equilibrium is a promising avenue to study their equilibrium properties as well as to control the superconducting state. Nonequilibrium superconductors are often studied using time-resolved optical conductivity measurements. Thus, the characterization of a superconducting state in a pump driven nonequilibrium state requires careful attention in the time domain. We calculate the time-resolved optical conductivity of a pumped superconducting state using a nonequilibrium Keldysh approach. Through functional derivation, the optical conductivity is obtained with full vertex corrections and used to characterize the transient superconducting state. The transient optical conductivity shows the suppression of the superconducting order parameter in the time domain. The subsequent recovery of the order parameter exhibits oscillatory behavior that corresponds to the Higgs amplitude mode, and may be seen in several parts of the spectrum.
This thesis reports on theoretical investigations of the ultrafast nonequilibrium dynamics in superconductors. In particular, two nonequilibrium scenarios are modeled by combining several analytical and numerical methods: transient superconducting phase transition and collective excitations of a superconducting condensate. In the first part of the thesis the possibility to induce singlet superconducting correlations far from equilibrium is explored by applying time-dependent Lanczos algorithm to the one-dimensional extended Hubbard model. Here, the system is driven into a nonequilibrium state by (i) interaction quench and (ii) quench by pulse. In both cases the buildup of the superconducting correlations is studied in view of several correlation functions. Moreover, a transient Meissner effect, which reflects fingerprints of the induced superconductivity, is observed in calculations of the important for experiments time-dependent optical conductivity. In addition, the differences between nonequilibrium dynamics of the extended Hubbard model initiated by interaction quench and by pulse quench are discussed in detail. The second part is devoted to the excitation of collective modes in a superconductor out of equilibrium. First of all, focus is given to the properties of collective modes close to equilibrium conditions, where a linearized response can be expected. Within the framework of the (Nambu-) matrix kinetic theory in the clean limit a comprehensive gauge-invariant description of the collective modes associated with phase fluctuations of the order parameter is analytically formulated for the generalized case of two- band superconducting systems. Particular emphasis is on the application to the recently discovered noncentrosymmetric superconductors. A detailed analysis of the collective modes includes specification of the gauge mode (common to all superconductors) and the Leggett mode (collective fluctuations of the interband phase difference), and investigation of their subtle interplay in view of validity of the charge conservation law and the participation in the Anderson-Higgs mechanism. Further, the nonequilibrium excitation of the superconducting gaps for the case of two-band superconductors with singlet pairing correlations is investigated in a view of optical pump-probe experiments. For this purpose a semi-numerical method based on the density- matrix theory is formulated. In this case additional amplitude (Higgs) modes were identified, which allow to directly detect the properties of the superconducting condensates as a function of time. Moreover, a new interplay between the phase (Leggett) and amplitude (Higgs) modes is studied in detail. In particular it was found that the nonadiabatic excitation process leads to strong coupling between both modes. Finally, based on calculations of the time-dependent optical conductivity the prediction is made that the coupled Higgs and Leggett modes can be clearly visible in the pump-probe absorption spectra.
Time-resolved optical conductivity is an often used tool to interrogate quantum materials driven out of equilibrium. Theoretically calculating this observable is a complex topic with several approaches discussed in the literature. Using a nonequilibrium Keldysh formalism and a functional derivative approach to the conductivity, we present a comparison of two particular approaches to the calculation of the optical conductivity and their distinguishing features, as applied to a pumped superconductor. The two methods are distinguished by the relative motion of the probe and gate times; either the probe or gate time is kept fixed while the other is swept. We find that both the methods result in same qualitative features of the time-resolved conductivity after pump is over. However, calculating the conductivity by keeping the gate fixed removes artifacts inherent to the other method. We provide software that, based on data for the first method, is able to construct the second approach.
We theoretically study the pump-probe response of nonequilibrium BCS superconductors coupled to optical phonons. For ultrashort pump pulses a nonadiabatic regime emerges, which is characterized by oscillations of the superconducting order parameter as well as by the generation of coherent phonons. Using the density-matrix formalism, we compute the pump-probe response in the nonadiabatic regime of the coupled Bogoliubov quasiparticle-phonon system and determine the signatures of the order parameter and the phonon oscillations in the pump-probe conductivity. We find that the nonadiabatic dynamics of the BCS superconductor reflects itself in oscillations of the pump-probe response as functions of delay time $\ensuremath{\delta}t$ between pump and probe pulses. We argue that from the analysis of this oscillatory behavior both frequency and decay time of the algebraically decaying order-parameter oscillations can be inferred. Similarly, the coherent phonons are evidenced in the pump-probe conductivity by oscillations with the frequency of the phonons. Remarkably, we find that the oscillatory response in the pump-probe conductivity is resonantly enhanced when the frequency of the order-parameter oscillations is tuned to the phonon energy.
Within the time-dependent Gutzwiller approximation applied to the negative-UUU Hubbard model, we investigate the dynamics of a superconductor after an interaction quench for different values of the final interaction from weak to strong coupling. The equilibrium BCS-BEC crossover becomes a sharp transition in the out-of-equilibrium dynamics between weak- and strong-coupling dynamical phases. Two different frequencies (${\mathrm{\ensuremath{\Omega}}}_{J}<{\mathrm{\ensuremath{\Omega}}}_{U}$) dominate the order parameter dynamics. In the weak coupling phase, ${\mathrm{\ensuremath{\Omega}}}_{J}$ follows twice the asymptotic average value of the gap (${\mathrm{\ensuremath{\Omega}}}_{J}\ensuremath{\approx}2{\mathrm{\ensuremath{\Delta}}}_{\ensuremath{\infty}}$) and ${\mathrm{\ensuremath{\Omega}}}_{U}$ is much larger but hardy visible in the anomalous density. At long times the BCS dynamics is recovered but surprisingly differences remain during the transient phase. In the strong coupling phase, the dynamics decouples from the asymptotic value of the order parameter except at exactly half filling and close to the dynamical transition where ${\mathrm{\ensuremath{\Omega}}}_{U}\ensuremath{\approx}2{\mathrm{\ensuremath{\Delta}}}_{\ensuremath{\infty}}$. The out-of-equilibrium transient spectral density and optical conductivity are presented and discussed in relation to pump probe experiments. Both ${\mathrm{\ensuremath{\Omega}}}_{J}$ and ${\mathrm{\ensuremath{\Omega}}}_{U}$ give rise to a complex structure of self-driven slow Rabi oscillations which are visible in the nonequilibrium optical conductivity where also sidebands appear due to the modulation of the double occupancy by superconducting amplitude oscillations. Analogous results apply to CDW and SDW systems. Our results show that in systems with long coherence times, pump-probe experiments allow us to characterize the regime (BCS vs preformed pairs) through very specific out-of-equilibrium fingerprints.
Cuprates are d-wave superconductors which exhibit a rich phase diagram: they are characterized by superconducting fluctuations even above the critical temperature, and thermal disorder can reduce or suppress the phase coherence. However, photoexcitation can have the opposite effect: recent experiments have shown an increasing phase coherence in optimally doped BSCCO with mid-infrared driving. Time-resolved terahertz spectroscopies are powerful techniques to excite and probe the non-equilibrium states of superconductors, directly addressing collective modes, such as amplitude (Higgs) oscillations. In this work, we calculate the full time evolution of the current generated by a cuprate with a quench-drive spectroscopy setup. Analyzing the response in Fourier space with respect to both the real time and the quench-drive delay time, we look for the signature of a transient modulation of higher harmonics, as well as the Higgs mode, in order to characterize the ground state phase. In particular, this approach can provide a smoking gun for induced or increased phase coherence when applied to the pseudogap phase. These results can pave the way for future experimental schemes to characterize and study superconductors alongside incoherent phases and phase transitions, including induced and transient superconductivity.
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.