Frequency-comb based double-quantum two-dimensional coherent spectroscopy identifies collective hyperfine resonances in atomic vapor induced by dipole-dipole interactions

Frequency comb based multidimensional coherent spectroscopy is a novel optical method that enables high resolution measurement in a short acquisition time. The method's resolution makes multidimensional coherent spectroscopy relevant for atomic systems that have narrow resonances. We use double-quantum multidimensional coherent spectroscopy to reveal collective hyperfine resonances in rubidium vapor at 100 C induced by dipole-dipole interactions. We observe tilted lineshapes in the double-quantum 2D spectra, which has never been reported for Doppler-broadened systems. The tilted lineshapes suggest that the signal is predominately from the interacting atoms that have near zero relative velocity

Spectroscopic Signatures of Electron-Phonon Coupling in Silicon-Vacancy Centers in Diamond

Vacancy centers in diamond have proven to be a viable solid-state platform for quantum coherent opto-electronic applications. Among the variety of vacancy centers, silicon-vacancy (SiV) centers have recently attracted much attention as an inversion-symmetric system that is less susceptible to electron-phonon interactions. Nevertheless, phonon-mediated processes still degrade the coherent properties of SiV centers, however characterizing their electron-phonon coupling is extremely challenging due to their weak spectroscopic signatures and remains an open experimental problem. In this paper we theoretically investigate signatures of electron-phonon coupling in simulated linear and nonlinear spectra of SiV centers. We demonstrate how even extremely weak electron-phonon interactions, such as in SiV centers, may be completely characterized via nonlinear spectroscopic techniques and even resolved between different fine-structure transitions

Frequency comb based four-wave-mixing spectroscopy

We experimentally demonstrate four-wave-mixing spectroscopy using frequency combs. The experiment uses a geometry where excitation pulses and four-wave-mixing signals generated by a sample co-propagate. We separate them in the radio frequency domain by heterodyne detection with a local oscillator comb that has a different repetition frequency

Comment on "Nonlinear fluctuations and dissipation in matter revealed by quantum light"

In a recent paper [Phys.~Rev.~A {\bf 91}, 053844 (2015)], Mukamel and Dorfman compare spectroscopies performed with classical vs.~quantum light, and conclude that \textit{nonlinear} quantum-spectroscopy signals cannot be obtained from averaging their classical-spectroscopy counterparts over the Glauber--Sudarshan quasiprobability distribution of the quantum field. In this Comment, we show that this interpretation is correct only if one assumes that a classical signal is given by a classical approximation for the field. While such an assumption can be useful for comparing theoretical results, it is never realized in laser spectroscopy experiments that typically use coherent states. Thus, instead of using classical signals, the connection between coherent states and quantum states of light must be considered. We rigorously show that quantum spectroscopy can always be projected from the experimentally realized coherent-state spectroscopy regardless how nonlinear the system response is.Comment: 4 page

Revealing and Characterizing Dark Excitons Through Coherent Multidimensional Spectroscopy

Dark excitons are of fundamental importance in a broad range of contexts, but are difficult to study using conventional optical spectroscopy due to their weak interaction with light. We show how coherent multidimensional spectroscopy can reveal and characterize dark states. Using this approach, we identify different types of dark excitons in InGaAs/GaAs quantum wells and determine details regarding lifetimes, homogeneous and inhomogeneous linewidths, broadening mechanisms and coupling strengths. The observations of coherent coupling between bright and dark excitons hint at a role for a multi-step process by which excitons in the barrier can relax into the quantum wells

Mode-Locked Chip Laser using Waveguide Arrays

We demonstrate theoretically that robust mode-locking can be achieved on a semiconductor chip with a waveguide array architecture. The waveguide arrays are used as an ideal saturable absorption mechanism for initial noise start-up as well as pulse shaping and stabilization. The cavity gain is provided by an injection current and forward biasing of the semiconductor material. The technology can be integrated directly with semiconductor architectures and technologies, thus allowing for the potential of an on-chip, broadband device.Comment: 3 pages, 3 figure

Two-dimensional Fourier-transform Spectroscopy of Potassium Vapor

Optical two-dimensional Fourier-transformed (2DFT) spectroscopy is used to study the coherent optical response of potassium vapor in a thin transmission cell. Rephasing and non-rephasing spectra of the D1 and D2 transitions are obtained and compared to numerical simulations. Calculations using the optical Bloch equations gives very good agreement with the experimental peak strengths and line shapes. Non-radiative Raman-like coherences are isolated using a different 2DFT projection. Density-dependent measurements show distortion of 2DFT spectra due to pulse propagation effects

Two-Dimensional Optical Spectroscopy of Excitons in Semiconductor Quantum Wells: Liouville-space pathway analysis

We demonstrate how dynamic correlations of heavy-hole and light-hole excitons in semiconductor quantum wells may be investigated by two dimensional correlation spectroscopy (2DCS). The coherent response to three femtosecond optical pulses is predicted to yield cross (off-diagonal) peaks that contain direct signatures of many-body two-exciton correlations. Signals generated at various phase-matching directions are compared.Comment: 27pages,13 figures, accepted for publication in Physical Review

Multidimensional Coherent Photocurrent Spectroscopy of a Semiconductor Nanostructure

Multidimensional Coherent Optical Photocurrent Spectroscopy (MD-COPS) is implemented using unstabilized interferometers. Photocurrent from a semiconductor sample is generated using a sequence of four excitation pulses in a collinear geometry. Each pulse is tagged with a unique radio frequency through acousto-optical modulation ; the Four-Wave Mixing (FWM) signal is then selected in the frequency domain. The interference of an auxiliary continuous wave laser, which is sent through the same interferometers as the excitation pulses, is used to synthesize reference frequencies for lock-in detection of the photocurrent FWM signal. This scheme enables the partial compensation of mechanical fluctuations in the setup, achieving sufficient phase stability without the need for active stabilization. The method intrinsically provides both the real and imaginary parts of the FWM signal as a function of inter-pulse delays. This signal is subsequently Fourier transformed to create a multi-dimensional spectrum. Measurements made on the excitonic resonance in a double InGaAs quantum well embedded in a p-i-n diode demonstrate the technique

Quantum-Well Laser Diodes for Frequency Comb Spectroscopy

We demonstrate simple optical frequency combs based on semiconductor quantum well laser diodes. The frequency comb spectrum can be tailored by choice of material properties and quantum-well widths, providing spectral flexibility. Finally, we demonstrate the mutual coherence of these devices by using two frequency combs on the same device to generate a radio-frequency dual comb spectrum