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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 WSe₂monolayer 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.

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.

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.

Quantum spectroscopy in solids directly detects nonlinear changes created exclusively by quantum fluctuations of light. So far, it has been realized only by projecting a large set of measurements with a coherent-state laser to a specific quantum-light response. We present two complementary experimental approaches to realize intense and ultrafast thermal-state sources. We investigate the effects of continuous excitation from a superluminescent diode (SLD) as well as an ensemble-averaging technique using phase-modulated pulses. By measuring excitonic nonlinearities in gallium arsenide, we demonstrate that the experimentally realized thermal-state source produces significantly reduced many-body nonlinearities compared to a coherent-state excitation. We also review experimental approaches toward future realization of quantum spectroscopy with thermal states.

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.

Optical multidimensional coherent spectroscopy (MDCS) is a nonlinear spectroscopy technique where a material is excited by a series of laser pulses to produce a spectrum as a function of multiple frequencies. The technique's ability to elucidate excited‐state structure and interactions has made MDCS a valuable tool in the study of excitons in semiconductors. This review introduces the method and describes progress it has fostered establishing a better understanding of dephasing rates, coherent coupling mechanisms, and many‐body interactions pertaining to optically generated electronic excitations in a variety of semiconductor material systems. Emphasis is placed on nanostructured gallium arsenide quantum wells and quantum dots, on quantum dots in other III–V and II–VI semiconductors, and on atomically thin transition metal dichalcogenides. Recent technical advances and potential future directions in the field are also discussed.