Quantum dynamics simulations of the 2D spectroscopy for exciton polaritons.

We develop an accurate and numerically efficient non-adiabatic path-integral approach to simulate the non-linear spectroscopy of exciton-polariton systems. This approach is based on the partial linearized density matrix approach to model the exciton dynamics with explicit propagation of the phonon bath environment, combined with a stochastic Lindblad dynamics approach to model the cavity loss dynamics. Through simulating both linear and polariton two-dimensional electronic spectra, we systematically investigate how light-matter coupling strength and cavity loss rate influence the optical response signal. Our results confirm the polaron decoupling effect, which is the reduced exciton-phonon coupling among polariton states due to the strong light-matter interactions. We further demonstrate that the polariton coherence time can be significantly prolonged compared to the electronic coherence outside the cavity.

Rapid multiplex ultrafast nonlinear microscopy for material characterization.

We demonstrate rapid imaging based on four-wave mixing (FWM) by assessing the quality of advanced materials through measurement of their nonlinear response, exciton dephasing, and exciton lifetimes. We use a WSe2 monolayer grown by chemical vapor deposition as a canonical example to demonstrate these capabilities. By comparison, we show that extracting material parameters such as FWM intensity, dephasing times, excited state lifetimes, and distribution of dark/localized states allows for a more accurate assessment of the quality of a sample than current prevalent techniques, including white light microscopy and linear micro-reflectance spectroscopy. We further discuss future improvements of the ultrafast FWM techniques by modeling the robustness of exponential decay fits to different spacing of the sampling points. Employing ultrafast nonlinear imaging in real-time at room temperature bears the potential for rapid in-situ sample characterization of advanced materials and beyond.

Coherent Interactions between Silicon-Vacancy Centers in Diamond.

We report tunable excitation-induced dipole-dipole interactions between silicon-vacancy color centers in diamond at cryogenic temperatures. These interactions couple centers into collective states, and excitation-induced shifts tag the excitation level of these collective states against the background of excited single centers. By characterizing the phase and amplitude of the spectrally resolved interaction-induced signal, we observe oscillations in the interaction strength and population state of the collective states as a function of excitation pulse area. Our results demonstrate that excitation-induced dipole-dipole interactions between color centers provide a route to manipulating collective intercenter states in the context of a congested, inhomogeneous ensemble.

Imaging dynamic exciton interactions and coupling in transition metal dichalcogenides.

Transition metal dichalcogenides (TMDs) are regarded as a possible material platform for quantum information science and related device applications. In TMD monolayers, the dephasing time and inhomogeneity are crucial parameters for any quantum information application. In TMD heterostructures, coupling strength and interlayer exciton lifetimes are also parameters of interest. However, many demonstrations in TMDs can only be realized at specific spots on the sample, presenting a challenge to the scalability of these applications. Here, using multi-dimensional coherent imaging spectroscopy, we shed light on the underlying physics-including dephasing, inhomogeneity, and strain-for a MoSe2 monolayer and identify both promising and unfavorable areas for quantum information applications. We, furthermore, apply the same technique to a MoSe2/WSe2 heterostructure. Despite the notable presence of strain and dielectric environment changes, coherent and incoherent coupling and interlayer exciton lifetimes are mostly robust across the sample. This uniformity is despite a significantly inhomogeneous interlayer exciton photoluminescence distribution that suggests a bad sample for device applications. This robustness strengthens the case for TMDs as a next-generation material platform in quantum information science and beyond.

High-speed hyperspectral four-wave-mixing microscopy with frequency combs.

A four-wave-mixing, frequency-comb-based, hyperspectral imaging technique that is spectrally precise and potentially rapid, and can in principle be applied to any material, is demonstrated in a near-diffraction-limited microscopy application.

Lock-in detector for accelerated nonlinear imaging.

We show that accelerated nonlinear imaging, such as stimulated Raman scattering and pump-probe imaging, is enabled by an order of magnitude reduction of data acquisition time when replacing the exponentially-weighted-moving-average low-pass filter in a lock-in amplifier with a simple-moving-average filter. We show that this simple-moving-average (box) lock-in yields a superior signal-to-noise ratio and suppression of extraneous modulations with short pixel dwell times, if one condition for the relation between the lock-in time constant and modulation frequencies is met. Our results, both theoretical and experimental, indicate that for nonlinear imaging applications, the box lock-in significantly outperforms conventional lock-in detection. These results facilitate the application of ultrafast and nonlinear imaging as a new standard for material characterization.

Hidden Silicon-Vacancy Centers in Diamond.

We characterize a high-density sample of negatively charged silicon-vacancy (SiV^{-}) centers in diamond using collinear optical multidimensional coherent spectroscopy. By comparing the results of complementary signal detection schemes, we identify a hidden population of SiV^{-} centers that is not typically observed in photoluminescence and which exhibits significant spectral inhomogeneity and extended electronic T_{2} times. The phenomenon is likely caused by strain, indicating a potential mechanism for controlling electric coherence in color-center-based quantum devices.

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. We demonstrate the correlation in the phase fluctuations between two devices on the same chip by generating a radio-frequency dual comb spectrum.

Fast phase cycling in non-collinear optical two-dimensional coherent spectroscopy.

As optical two-dimensional coherent spectroscopy (2DCS) is extended to a broader range of applications, it is critical to improve the detection sensitivity of optical 2DCS. We developed a fast phase-cycling scheme in a non-collinear optical 2DCS implementation by using liquid crystal phase retarders to modulate the phases of two excitation pulses. The background in the signal can be eliminated by combining either two or four interferograms measured with a proper phase configuration. The effectiveness of this method was validated in optical 2DCS measurements of an atomic vapor. This fast phase-cycling scheme will enable optical 2DCS in novel emerging applications that require enhanced detection sensitivity.

Effect of dimensionality on the optical absorption properties of CsPbI3 perovskite nanocrystals.

The bandgaps of CsPbI3 perovskite nanocrystals are measured by absorption spectroscopy at cryogenic temperatures. Anomalous bandgap shifts are observed in CsPbI3 nanocubes and nanoplatelets, which are modeled accurately by bandgap renormalization due to lattice vibrational modes. We find that decreasing dimensionality of the CsPbI3 lattice in nanoplatelets greatly reduces electron-phonon coupling, and dominant out-of-plane quantum confinement results in a homogeneously broadened absorption line shape down to cryogenic temperatures. An absorption tail forms at low-temperatures in CsPbI3 nanocubes, which we attribute to shallow defect states positioned near the valence band edge.

Optimum repetition rates for dual-comb spectroscopy.

The determination of the properties (i.e. line center, width, and amplitude) of a spectral line is simulated using a Monte Carlo method. For dual-comb spectroscopy, ideal repetition rates emerge for both the signal and LO combs that do not correspond to the repetition rates that possess the highest signal-to-noise ratio. The determination is even more accurate when the repetition rates have an arbitrary near-harmonic ratio. The simulation results are generalized to allow for the comparison of any two spectroscopic systems (i.e. not just comb-based systems) by performing the simulations as a function of the spectral point spacing and signal-to-noise ratio of the acquired data.

Frequency-Comb Based Double-Quantum Two-Dimensional Spectrum 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 and elongated line shapes in the double-quantum 2D spectra, which have never been reported for Doppler-broadened systems. The elongated line shapes suggest that the signal is predominately from the interacting atoms that have a near zero relative velocity.

Frequency comb-based four-wave-mixing spectroscopy.

We experimentally demonstrate four-wave-mixing (FWM) spectroscopy using frequency combs. The experiment uses a geometry where excitation pulses and FWM 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.

Probing dipole-dipole interaction in a rubidium gas via double-quantum 2D spectroscopy.

We have implemented double-quantum 2D spectroscopy on a rubidium vapor and shown that this technique provides sensitive and background-free detection of the dipole-dipole interaction. The 2D spectra include signals from both individual atoms and interatomic interactions, allowing quantitative studies of the interaction. A theoretical model based on the optical Bloch equations is used to reproduce the experimental spectrum and confirm the origin of double-quantum signals.

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 parity-forbidden and spatially indirect 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 these states and bright excitons hint at a role for a multistep process by which excitons in the barrier can relax into the quantum wells.

Coherent Control of the Exciton-Biexciton System in an InAs Self-Assembled Quantum Dot Ensemble.

Coherent control of a strongly inhomogeneously broadened system, namely, InAs self-assembled quantum dots, is demonstrated. To circumvent the deleterious effects of the inhomogeneous broadening, which usually masks the results of coherent manipulation, we use prepulse two-dimensional coherent spectroscopy to provide a size-selective readout of the ground, exciton, and biexciton states. The dependence on the timing of the prepulse is due to the dynamics of the coherently generated populations. To further validate the results, we performed prepulse polarization dependent measurements and confirmed the behavior expected from selection rules. All measured spectra can be excellently reproduced by solving the optical Bloch equations for a 4-level system.

Observation of Coexisting Dissipative Solitons in a Mode-Locked Fiber Laser.

We show, experimentally and numerically, that a mode-locked fiber laser can operate in a regime where two dissipative soliton solutions coexist and the laser will periodically switch between the solutions. The two dissipative solitons differ in their pulse energy and spectrum. The switching can be controlled by an external perturbation and triggered even when switching does not occur spontaneously. Numerical simulations unveil the importance of the double-minima loss spectrum and nonlinear gain to the switching dynamics.

Pulse Propagation Effects in Optical 2D Fourier-Transform Spectroscopy: Theory.

A solution to Maxwell's equations in the three-dimensional frequency domain is used to calculate rephasing two-dimensional Fourier transform (2DFT) spectra of the D2 line of atomic rubidium vapor in argon buffer gas. Experimental distortions from the spatial propagation of pulses through the sample are simulated in 2DFT spectra calculated for the homogeneous Bloch line shape model. Spectral features that appear at optical densities of up to 3 are investigated. As optical density increases, absorptive and dispersive distortions start with peak shape broadening, progress to peak splitting, and ultimately result in a previously unexplored coherent transient twisting of the split peaks. In contrast to the low optical density limit, where the 2D peak shape for the Bloch model depends only on the total dephasing time, these distortions of the 2D peak shape at finite optical density vary with the waiting time and the excited state lifetime through coherent transient effects. Experiment-specific conditions are explored, demonstrating the effects of varying beam overlap within the sample and of pseudo-time domain filtering. For beam overlap starting at the sample entrance, decreasing the length of beam overlap reduces the line width along the ωτ axis but also reduces signal intensity. A pseudo-time domain filter, where signal prior to the center of the last excitation pulse is excluded from the FID-referenced 2D signal, reduces propagation distortions along the ωt axis. It is demonstrated that 2DFT rephasing spectra cannot take advantage of an excitation-detection transformation that can eliminate propagation distortions in 2DFT relaxation spectra. Finally, the high optical density experimental 2DFT spectrum of rubidium vapor in argon buffer gas [J. Phys. Chem. A 2013, 117, 6279-6287] is quantitatively compared, in line width, in depth of peak splitting, and in coherent transient peak twisting, to a simulation with optical density higher than that reported.

Pulse dynamics in a mode-locked fiber laser and its quantum limited comb frequency uncertainty.

We present an experimental study of pulse dynamics in a mode-locked Er:fiber laser. By injecting a continuous wave laser with sinusoidal intensity modulation into the fiber laser, we are able to modulate the gain. Measuring the response of the pulse energy, central frequency, central pulse time, and phase to the gain modulation allows determination of the parameters that describe their coupling. Based on the experimentally derived parameters, we evaluate the free running comb linewidth and frequency uncertainty with feedback included, assuming quantum noise is the limiting factor. Optimization of fiber lasers is also discussed.