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arXiv:2306.11998 · Physical review. B./Physical review. B

Microscopic many-body theory of two-dimensional coherent spectroscopy of exciton polarons in one-dimensional materials

Jia Wang, Hui Hu, Xia-Ji Liu

Published May 13, 2024• 0 citations
arXivHTMLPDF

Abstract

We have developed a microscopic many-body theory of two-dimensional coherent spectroscopy (2DCS) for a model of polarons in one-dimensional (1D) materials. Our theory accounts for contributions from all three processes: excited-state emission (ESE), ground-state bleaching (GSB), and excited-state absorption (ESA). While the ESE and GSB contributions can be accurately described using Chevy's ansatz with one-particle-hole excitation, the ESA process requires information about the many-body eigenstates involving two impurities. To calculate these double polaron states, we have extended Chevy's ansatz with one-particle-hole excitation. The validity of this ansatz was verified by comparing our results with an exact calculation using Bethe's ansatz. Our numerical results reveal that in, the weak interaction limit, the ESA contribution cancels out the total ESE and GSB contributions, resulting in less significant spectral features. However, for strong interactions, the features of the ESA contribution and the combined ESE and GSB contributions remain observable in the 2DCS spectra. These features provide valuable information about the interactions between polarons. Additionally, we have investigated the mixing time dynamics, which characterize the quantum coherences of the polaron resonances. Overall, our theory provides a comprehensive framework for understanding and interpreting the 2DCS spectra of polarons in 1D materials, shedding light on their interactions and coherent dynamics.

DOI
10.1103/physrevb.109.205414

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We have developed a microscopic many-body theory of two-dimensional coherent spectroscopy (2DCS) for a model of polarons in one-dimensional (1D) materials. Our theory accounts for contributions from all three processes: excited-state emission (ESE), ground-state bleaching (GSB), and excited-state absorption (ESA). While the ESE and GSB contributions can be accurately described using Chevy's ansatz with one-particle-hole excitation, the ESA process requires information about the many-body eigenstates involving two impurities. To calculate these double polaron states, we have extended Chevy's ansatz with one-particle-hole excitation. The validity of this ansatz was verified by comparing our results with an exact calculation using Bethe's ansatz. Our numerical results reveal that in, the weak interaction limit, the ESA contribution cancels out the total ESE and GSB contributions, resulting in less significant spectral features. However, for strong interactions, the features of the ESA contribution and the combined ESE and GSB contributions remain observable in the 2DCS spectra. These features provide valuable information about the interactions between polarons. Additionally, we have investigated the mixing time dynamics, which characterize the quantum coherences of the polaron resonances. Overall, our theory provides a comprehensive framework for understanding and interpreting the 2DCS spectra of polarons in 1D materials, shedding light on their interactions and coherent dynamics.
Multidimensional spectroscopy is becoming an increasingly popular tool and there is an ongoing effort to access electronic transitions and many-body dynamics in correlated materials. We apply the protocol recently proposed by Wang [Phys. Rev. A 107, 013305 (2023)] to extract two-dimensional polaron spectra in a Fermi superfluid with an impurity. The bath is described by a BCS ansatz and it assumed that the impurity can scatter at most one quasiparticle pair. The spectral response contains a symmetric contribution, which carries the same information as Ramsey spectra, and an asymmetric one. While a priori it may seem promising to probe the quasiparticle gap from the asymmetric contribution, we show explicitly that this is not the case and, in the absence of incoherent processes, multidimensional spectroscopy does not bring much additional information. Our calculation is suitable for ultracold gases, but we discuss implications for exciton polarons in two-dimensional materials.
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It has been commonly believed that a polaron-to-molecule transition occurs in three-dimensional (3D) and 2D Fermi polaron systems as the attraction between the single impurity and majority fermions gets stronger. The conclusion has been drawn from the separate treatment of polaron and molecule states and thus deserves a close reexamination. In this work, we explore the physics of polarons and molecules by utilizing a unified variational Ansatz with up to two particle-hole (ph) excitations (V-2ph). We confirm the existence of a first-order transition in 3D and 2D Fermi polarons, and we show that the nature of such a transition lies in an energy competition between systems with different momenta, $\mathbf{Q}=\mathbit{0}$ and ∣Q∣=kF|\mathbf{Q}|={k}_{F}∣Q∣=kF​; here Q\mathbf{Q}Q is defined as the momentum of a Fermi polaron system with respect to the Fermi sea of majority fermions (with Fermi momentum kF{k}_{F}kF​). The literally proposed molecule Ansatz is identified as an asymptotic limit of the ∣Q∣=kF|\mathbf{Q}|={k}_{F}∣Q∣=kF​ state in a strong-coupling regime, which implies a huge SO(3)\text{SO}(3)SO(3) (for 3D) or SO(2)\text{SO}(2)SO(2) (for 2D) ground-state degeneracy in this regime. The recognition of such degeneracy is crucially important for evaluating the molecule occupation in realistic systems with finite impurity density and at finite temperature. To compare with recent experiment of 3D Fermi polarons, we have calculated various physical quantities under the V-2ph framework, and we obtained results that are in good agreement with experimental data in the weak-coupling and near-resonance regime. Further, to check the validity of our conclusion in 2D, we have adopted a different variational method based on the Gaussian sample of high-order ph excitations (V-Gph), and we found the same conclusion on the nature of the polaron-molecule transition therein. For a 1D system, the V-2ph method predicts no sharp transition, and the ground state is always at the $\mathbf{Q}=\mathbit{0}$ sector, consistent with the exact Bethe-Ansatz solution. The presence/absence of a polaron-molecule transition is analyzed to be closely related to the interplay effect of Pauli-blocking and ph excitations in different dimensions.
We develop a general theory of Fermi polarons at nonzero temperature, including particle-hole excitations of the Fermi sea shakeup to arbitrarily high orders. The exact set of equations of the spectral function is derived by using both Chevy ansatz and diagrammatic approach, and their equivalence is clarified to hold in free space only, with an unregularized infinitesimal interaction strength. The correction to the polaron spectral function arising from two-particle-hole excitations is explicitly examined for an exemplary case of Fermi polarons in one-dimensional optical lattices. We find quantitative improvements at low temperatures with the inclusion of two-particle-hole excitations, in both polaron energies and decay rates. Our exact theory of Fermi polarons with arbitrary orders of particle-hole excitations might be used to better understand the intriguing polaron dynamical responses in two or three dimensions, whether in free space or within lattices.
An exact-diagonalization technique is used to investigate the low-lying excited polaron states in the Holstein model for the infinite one-dimensional lattice. For moderate values of the adiabatic ratio, a comprehensive picture, involving three excited (coherent) polaron bands below the phonon threshold, is obtained. The coherent contribution of the excited states to both the single-electron spectral density and the optical conductivity is evaluated and, due to the invariance of the Hamiltonian under the space inversion, the two are shown to contain complementary information about the single-electron system at zero temperature. The chosen method reveals the connection between the excited bands and the renormalized local phonon excitations of the adiabatic theory, as well as the regime of parameters for which the electron self-energy has notable nonlocal contributions. Finally, it is shown that the hybridization of two polaron states allows a simple description of the ground and first excited states in the crossover regime.
Abstract By using both diagrammatic theory and Chevy ansatz approach, we derive an exact set of equations, which determines the spectral function of Fermi polarons with multiple particle-hole excitations at nonzero temperature. In the diagrammatic theory, we find out the complete series of Feynman diagrams for the multi-particle vertex functions, when the unregularized contact interaction strength becomes infinitesimal, a typical situation occurring in two- or three-dimensional free space. The latter Chevy ansatz approach is more widely applicable, allowing a nonzero interaction strength. We clarify the equivalence of the two approaches for an infinitesimal interaction strength and show that the variational coefficients in the Chevy ansatz are precisely the on-shell multi-particle vertex functions divided by an excitation energy. Truncated to a particular order of particle-hole excitations, the set of equations can be used to approximately calculate the finite-temperature polaron spectral function, once the numerical singularities in the equations are appropriately treated. As a concrete example, we calculate the finite-temperature spectral function of Fermi polarons in one-dimensional lattices, taking into account all the two-particle-hole excitations. We show that the inclusion of two-particle-hole excitations quantitatively improve the predictions on the polaron spectral function. Our results provide a useful way to solve the challenge problem of accurately predicting the finite-temperature spectral function of Fermi polarons in three-dimensional free space. In addition, our clarification of the complete set of Feynman diagrams for the multi-particle polaron vertex functions may inspire the development of more accurate diagrammatic theories of population-imbalanced strongly interacting Fermi gases, beyond the conventional many-body T-matrix approximation.