Absorption band shapes of an asymmetric dimer system constituted by monomers with different excitation energies and optical transition matrix elements are considered in the semiclassical parameter region. Optical transition matrix elements originating from arbitrary initial vibrational states are analyzed on the basis of a spin representation of the eigenstates of an associated symmetry broken spin-boson Hamiltonian. Correlations between the spin-down and spin-up coefficients of these eigenstates are shown to exist and investigated in detail. Using these correlations, an asymmetry interpolation of the intensity of absorption lines between dimer configurations with different optical monomer transition matrix elements is proposed.
We consider three distinct methods of calculating the vibronic levels and absorption spectra of molecular dimers coupled by dipole-dipole interactions. The first method is direct diagonalization of the vibronic Hamiltonian in a basis of monomer eigenstates. The second method is to use creation and annihilation operators leading in harmonic approximation to the Jaynes-Cummings Hamiltonian. The adiabatic approximation to this problem provides insight into spectral behavior in the weak and strong coupling limits. The third method, which serves as a check on the accuracy of the previous methods, is a numerically exact solution of the time-dependent Schrodinger equation. Using these methods, dimer spectra are calculated for three separate dye molecules and show good agreement with measured spectra.
We theoretically investigate the light absorption spectrum of two-dimensional (2D) Mott insulators. We employ the numerical diagonalization method to calculate the light absorption spectrum with using the effective Hamiltonian for the extended Hubbard model, which is valid when the on-site Coulomb interaction energy
U is much larger than the nearest-neighbor transfer integral
t and the nearest-neighbor Coulomb interaction energy
V. For
V=0, the absorption spectrum consists of a broad band with a width of about
16t and a sharp central peak, and the energy eigenstates contributing to the absorption spectrum do not have the antiferromagnetic (AF) spin order, when
U is sufficiently larger than
t. These features result from the spin-charge interplay inherent in the very strong correlation region where charge transfer term is dominant. With decreasing
U∕t, the peak structure in absorption spectrum becomes unclear and some low energy eigenstates have the AF spin order, as a result of the spin-spin interaction term. For large
V∕t, the dominant peak arises in the lower energy region of the spectrum. A large number of holon-doublon bound states, which have nearly the same charge but different spin structures, are responsible for this peak, in contrast to the conventional exciton state. This is also in contrast to the charge bound states in one-dimensional (1D) Mott insulators, where a single energy eigenstate dominates the optical transition moment as a result of the spin-charge separation. The essentially different absorption spectra between the 1D and 2D Mott insulators originate from the difference in the coupling between spin and charge degrees of freedom.
The extended effective multiorbital Bose–Hubbard-type Hamiltonian which takes into account higher Bloch bands is discussed for boson systems in optical lattices, with emphasis on dynamical properties, in relation to current experiments. It is shown that the renormalization of Hamiltonian parameters depends on the dimension of the problem studied. Therefore, mean-field phase diagrams do not scale with the coordination number of the lattice. The effect of Hamiltonian parameters renormalization on the dynamics in reduced one-dimensional optical lattice potential is analyzed. We study both the quasi-adiabatic quench through the superfluid–Mott insulator transition and the absorption spectroscopy, that is, the energy absorption rate when the lattice depth is periodically modulated.
The energy band structure of spin-1 condensates with repulsive spin-independent and either ferromagnetic or antiferromagnetic spin-dependent interactions in one-dimensional (1D) periodic optical lattices is discussed. Within the two-mode approximation, Bloch bands of spin-1 condensates are presented. The results show that the Bloch bands exhibit a complex structure as the atom density of mF = 0 hyperfine state increases: bands splitting, reversion, intersection and loop structure are excited subsequently. The complex band structure should be related to the tunneling and spin-mixing dynamics.
Lie algebra, Zassenhaus, and parameter differentiation techniques are utilized to break up the exponential of a bilinear Hamiltonian operator into a product of noncommuting exponential operators by the virtue of the theory of Wei and Norman [J. Math. Phys. 4, 575 (1963); Proc. Am. Math. Soc., 15, 327 (1964)]. There are about three different ways to find the Zassenhaus exponents, namely, binomial expansion, Suzuki formula, and q-exponential transformation. A fourth, and most reliable method, is provided. Since linearly displaced and distorted (curvature change upon excitation/emission) Hamiltonian and spin-boson Hamiltonian may be classified as bilinear Hamiltonians, the presented algebraic algorithm (exponential operator disentanglement exploiting six-dimensional Lie algebra case) should be useful in spin-boson problems. The linearly displaced and distorted Hamiltonian exponential is only treated here. While the spin-boson model is used here only as a demonstration of the idea, the herein approach is more general and powerful than the specific example treated. The optical linear dipole moment correlation function is algebraically derived using the above mentioned methods and coherent states. Coherent states are eigenvectors of the bosonic lowering operator a and not of the raising operator a(+). While exp(a(+)) translates coherent states, exp(a(+)a(+)) operation on coherent states has always been a challenge, as a(+) has no eigenvectors. Three approaches, and the results, of that operation are provided. Linear absorption spectra are derived, calculated, and discussed. The linear dipole moment correlation function for the pure quadratic coupling case is expressed in terms of Legendre polynomials to better show the even vibronic transitions in the absorption spectrum. Comparison of the present line shapes to those calculated by other methods is provided. Franck-Condon factors for both linear and quadratic couplings are exactly accounted for by the herein calculated linear absorption spectra. This new methodology should easily pave the way to calculating the four-point correlation function, F(tau(1),tau(2),tau(3),tau(4)), of which the optical nonlinear response function may be procured, as evaluating F(tau(1),tau(2),tau(3),tau(4)) is only evaluating the optical linear dipole moment correlation function iteratively over different time intervals, which should allow calculating various optical nonlinear temporal/spectral signals.