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Register a new userMicroscopic Theory for the Incoherent Resonant and Coherent Off-Resonant Optical Response of Tellurium
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An $it{ab ,, initio}$ based fully microscopic approach is applied to study the nonlinear optical response of bulk Tellurium. The structural and electronic properties are calculated from first principles using the shLDA-1/2 method within density functional theory. The resulting bandstructure and dipole matrix elements serve as input for the quantum mechanical evaluation of the anisotropic linear optical absorption spectra yielding results in excellent agreement with published experimental data. Assuming quasi-equilibrium carrier distributions in the conduction and valence bands, absorption/gain and spontaneous emission spectra are computed from the semiconductor Bloch and luminescence equations. For ultrafast intense off-resonant excitation, the generation of high-harmonics is evaluated and the emission spectra are calculated for samples of different thickness.
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Three-color coherent anti-Stokes Raman scattering represents non-degenerate four wave mixing process that includes both a non-resonant and resonant processes, the contributions of which depend on how the molecular vibrational modes are being excited by the input laser pulses. Non-degenerate four wave mixing processes are complex and understanding these processes requires rigorous data analytical tools, which still lack in this research field. In this work, we introduce one- and two-dimensional intensity-intensity correlation functions in terms of a new variable (e.g., probe pulse delay) and new perturbation parameter (e.g., probe pulse linewidth). In particular, diagonal projections are defined here as a tool to reduce both synchronous and asynchronous two-dimensional correlation spectroscopy analyses down to one-dimensional analysis, revealing valuable analytical information. Detailed analyses using the all Gaussian coherent Raman scattering closed-form solutions and the representative experimental data for resonant and non-resonant processes are presented and compared. This intensity-intensity correlation analytical tool holds a promising potential in resolving and visualizing resonant versus non-resonant four wave mixing processes for quantitative label-free species-specific nonlinear spectroscopy and microscopy.
A convenient for practical use new theoretical approach describing a nonlinear frequency response of the multi-resonant nonlinear ring cavities (RC) to an intense monochromatic wave action is developed. The approach closely relates the many-valuednesses of the RC frequency response and the dispersion relation of a waveguide, from which the cavity is produced. Arising of the multistability regime in the nonlinear RC is treated. The threshold and the dynamic range of the bistability and tristability regimes for an optical ring cavity with the Kerr nonlinearity are derived and discussed.
The theory of incoherent nuclear resonant scattering of synchrotron radiation accompanied by absorption or emission of phonons in a crystal lattice is developed. The theory is based on the Maxwells equations and time-dependent quantum mechanics under the condition of incoherent scattering of radiation by various nuclei. A concept of coherence in scattering processes, properties of the synchrotron radiation, and conditions of measurement are discussed. We show that employing the monochromator with a narrow bandwidth plays a decisive role.
Optical cavities are a cornerstone of photonics. They are indispensable in lasers, optical filters, optical combs and clocks, in quantum physics, and have enabled the detection of gravitational waves. Cavities transmit light only at discrete resonant frequencies, which are well-separated in micro-structures. Despite attempts at the construction of `white-light cavities, the benefits accrued upon optically interacting with a cavity -- such as resonant field buildup -- have remained confined to narrow linewidths. Here, we demonstrate achromatic optical transmission through a planar Fabry-Perot micro-cavity via angularly multiplexed phase-matching that exploits a bio-inspired grating configuration. By correlating each wavelength with an appropriate angle of incidence, a continuous spectrum resonates and the micro-cavity is rendered transparent. The locus of a single-order 0.7-nm-wide resonance is de-slanted in spectral-angular space to become a 60-nm-wide achromatic resonance spanning multiple cavity free-spectral-ranges. This approach severs the link between the resonance bandwidth and the cavity-photon lifetime, thereby promising resonant enhancement of linear and nonlinear optical effects over broad bandwidths in ultrathin devices.
Coherent perfect absorption (CPA) refers to interferometrically induced complete absorption of incident light by a partial absorber independently of its intrinsic absorption (which may be vanishingly small) or its thickness. CPA is typically realized in a resonant device, and thus cannot be achieved over a broad continuous spectrum, which thwarts its applicability to photodetectors and solar cells, for example. Here, we demonstrate broadband omni-resonant CPA by placing a thin weak absorber in a planar cavity and pre-conditioning the incident optical field by introducing judicious angular dispersion. We make use of monolayer graphene embedded in silica as the absorber and boost its optical absorption from ~1.6% to ~60% over a bandwidth of ~70 nm in the visible. Crucially, an analytical model demonstrates that placement of the graphene monolayer at a peak in the cavity standing-wave field is not necessary to achieve CPA, contrary to conventional wisdom.
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