2021 Vol. 10, No. 12
Published. 2021, 10(12)
: 2249-2255
doi: 10.1038/s41377-021-00673-9
He pioneered a new family of nanoscopic probes that can up-convert infrared photons into intense visible light, and won the Australian Museum Eureka Prize for Interdisciplinary Scientific Research in 2015. He created new kinds of microscopes that allow us to watch molecules at work inside living cells, and won the Australian Prime Minister's Prize for Science Malcolm McIntosh Prize for Physical Scientist of the Year 2017. The Australian newspaper identified him among 100 "rock stars of Australia's new economy" as the Knowledge Nation 100. This year, at his age of 42, he won the Australian Laureate Fellowship and was elected to the fellowship of Australian Academy of Technology and Engineering. This is Dayong Jin, a Distinguished Professor at the University of Technology Sydney and a Chair Professor at Southern University of Science and Technology, as well as the editorial manager in Sydney office and the perspective column editor of Light: Science & Applications (LSA). Light People is a featured column of high-end interviews with outstanding scientists. On this issue, it is our great honor to invite Professor Dayong Jin to provide his perspectives on his work, end-user driven research, student mentoring and team building philosophy. In the following, let's take a closer look at the research life of Professor Dayong Jin, and appreciate his style and the story behind his success.
Published. 2021, 10(12)
: 2256-2257
doi: 10.1038/s41377-021-00656-w
The intra-cavity electro-magnetic field distribution in a microdisk resonator can be visualised by inducing a phase shift via a scanning probe beam.
Published. 2021, 10(12)
: 2258-2260
doi: 10.1038/s41377-021-00684-6
Highly sensitive force measurements of a single microscopic particle with femto-Newton sensitivity have remained elusive owing to the existence of fundamental thermal noise. Now, researchers have proposed an optically controlled hydrodynamic manipulation method, which can measure the weak force of a single microscopic particle with femto-Newton sensitivity.
Published. 2021, 10(12)
: 2263-2306
doi: 10.1038/s41377-021-00655-x
The growing maturity of nanofabrication has ushered massive sophisticated optical structures available on a photonic chip. The integration of subwavelength-structured metasurfaces and metamaterials on the canonical building block of optical waveguides is gradually reshaping the landscape of photonic integrated circuits, giving rise to numerous meta-waveguides with unprecedented strength in controlling guided electromagnetic waves. Here, we review recent advances in meta-structured waveguides that synergize various functional subwavelength photonic architectures with diverse waveguide platforms, such as dielectric or plasmonic waveguides and optical fibers. Foundational results and representative applications are comprehensively summarized. Brief physical models with explicit design tutorials, either physical intuition-based design methods or computer algorithms-based inverse designs, are cataloged as well. We highlight how meta-optics can infuse new degrees of freedom to waveguide-based devices and systems, by enhancing light-matter interaction strength to drastically boost device performance, or offering a versatile designer media for manipulating light in nanoscale to enable novel functionalities. We further discuss current challenges and outline emerging opportunities of this vibrant field for various applications in photonic integrated circuits, biomedical sensing, artificial intelligence and beyond.
Published. 2021, 10(12)
: 2307-2321
doi: 10.1038/s41377-021-00670-y
We review results on the optical injection of dual state InAs quantum dot-based semiconductor lasers. The two states in question are the so-called ground state and first excited state of the laser. This ability to lase from two different energy states is unique amongst semiconductor lasers and in combination with the high, intrinsic relaxation oscillation damping of the material and the novel, inherent cascade like carrier relaxation process, endows optically injected dual state quantum dot lasers with many unique dynamical properties. Particular attention is paid to fast state switching, antiphase excitability, novel information processing techniques and optothermally induced neuronal phenomena. We compare and contrast some of the physical properties of the system with other optically injected two state devices such as vertical cavity surface emitting lasers and ring lasers. Finally, we offer an outlook on the use of quantum dot material in photonic integrated circuits.
Published. 2021, 10(12)
: 2322-2329
doi: 10.1038/s41377-021-00634-2
Quantum secure direct communication (QSDC) based on entanglement can directly transmit confidential information. However, the inability to simultaneously distinguish the four sets of encoded entangled states limits its practical application. Here, we explore a QSDC network based on time–energy entanglement and sum-frequency generation. In total, 15 users are in a fully connected QSDC network, and the fidelity of the entangled state shared by any two users is > 97%. The results show that when any two users are performing QSDC over 40 km of optical fiber, the fidelity of the entangled state shared by them is still > 95%, and the rate of information transmission can be maintained above 1 Kbp/s. Our result demonstrates the feasibility of a proposed QSDC network and hence lays the foundation for the realization of satellite-based long-distance and global QSDC in the future.
Published. 2021, 10(12)
: 2330-2341
doi: 10.1038/s41377-021-00666-8
Optical implementations of neural networks (ONNs) herald the next-generation high-speed and energy-efficient deep learning computing by harnessing the technical advantages of large bandwidth and high parallelism of optics. However, due to the problems of the incomplete numerical domain, limited hardware scale, or inadequate numerical accuracy, the majority of existing ONNs were studied for basic classification tasks. Given that regression is a fundamental form of deep learning and accounts for a large part of current artificial intelligence applications, it is necessary to master deep learning regression for further development and deployment of ONNs. Here, we demonstrate a silicon-based optical coherent dot-product chip (OCDC) capable of completing deep learning regression tasks. The OCDC adopts optical fields to carry out operations in the complete real-value domain instead of in only the positive domain. Via reusing, a single chip conducts matrix multiplications and convolutions in neural networks of any complexity. Also, hardware deviations are compensated via in-situ backpropagation control provided the simplicity of chip architecture. Therefore, the OCDC meets the requirements for sophisticated regression tasks and we successfully demonstrate a representative neural network, the AUTOMAP (a cutting-edge neural network model for image reconstruction). The quality of reconstructed images by the OCDC and a 32-bit digital computer is comparable. To the best of our knowledge, there is no precedent of performing such state-of-the-art regression tasks on ONN chips. It is anticipated that the OCDC can promote the novel accomplishment of ONNs in modern AI applications including autonomous driving, natural language processing, and scientific study.
Published. 2021, 10(12)
: 2342-2348
doi: 10.1038/s41377-021-00663-x
Measuring the aberrations of optical systems is an essential step in the fabrication of high precision optical components. Such a characterization is usually based on comparing the device under investigation with a calibrated reference object. However, when working at the cutting-edge of technology, it is increasingly difficult to provide an even better or well-known reference device. In this manuscript we present a method for the characterization of high numerical aperture microscope objectives, functioning without the need of calibrated reference optics. The technique constitutes a nanoparticle, acting as a dipole-like scatterer, that is placed in the focal volume of the microscope objective. The light that is scattered by the particle can be measured individually and serves as the reference wave in our system. Utilizing the well-characterized scattered light as nearly perfect reference wave is the main idea behind this manuscript.
Published. 2021, 10(12)
: 2349-2359
doi: 10.1038/s41377-021-00664-w
Optical imaging is a most useful and widespread technique for the investigation of the structure and function of the cellular genomes. However, an analysis of immensely convoluted and irregularly compacted DNA polymer is highly challenging even by modern super-resolution microscopy approaches. Here we propose fluorescence lifetime imaging (FLIM) for the advancement of studies of genomic structure including DNA compaction, replication as well as monitoring of gene expression. The proposed FLIM assay employs two independent mechanisms for DNA compaction sensing. One mechanism relies on the inverse quadratic relation between the fluorescence lifetimes of fluorescence probes incorporated into DNA and their local refractive index, variable due to DNA compaction density. Another mechanism is based on the Förster resonance energy transfer (FRET) process between the donor and the acceptor fluorophores, both incorporated into DNA. Both these proposed mechanisms were validated in cultured cells. The obtained data unravel a significant difference in compaction of the gene-rich and gene-poor pools of genomic DNA. We show that the gene-rich DNA is loosely compacted compared to the dense DNA domains devoid of active genes.
Published. 2021, 10(12)
: 2360-2368
doi: 10.1038/s41377-021-00667-7
The emergence of cylindrical vector beam (CVB) multiplexing has opened new avenues for high-capacity optical communication. Although several configurations have been developed to couple/separate CVBs, the CVB multiplexer/demultiplexer remains elusive due to lack of effective off-axis polarization control technologies. Here we report a straightforward approach to realize off-axis polarization control for CVB multiplexing/demultiplexing based on a metal–dielectric–metal metasurface. We show that the left- and right-handed circularly polarized (LHCP/RHCP) components of CVBs are independently modulated via spin-to-orbit interactions by the properly designed metasurface, and then simultaneously multiplexed and demultiplexed due to the reversibility of light path and the conservation of vector mode. We also show that the proposed multiplexers/demultiplexers are broadband (from 1310 to 1625 nm) and compatible with wavelength-division-multiplexing. As a proof of concept, we successfully demonstrate a four-channel CVB multiplexing communication, combining wavelength-division-multiplexing and polarization-division-multiplexing with a transmission rate of 1.56 Tbit/s and a bit-error-rate of 10−6 at the receive power of −21.6 dBm. This study paves the way for CVB multiplexing/demultiplexing and may benefit high-capacity CVB communication.
Published. 2021, 10(12)
: 2369-2379
doi: 10.1038/s41377-021-00665-9
Various biological behaviors can only be observed in 3D at high speed over the long term with low phototoxicity. Light-field microscopy (LFM) provides an elegant compact solution to record 3D information in a tomographic manner simultaneously, which can facilitate high photon efficiency. However, LFM still suffers from the missing-cone problem, leading to degraded axial resolution and ringing effects after deconvolution. Here, we propose a mirror-enhanced scanning LFM (MiSLFM) to achieve long-term high-speed 3D imaging at super-resolved axial resolution with a single objective, by fully exploiting the extended depth of field of LFM with a tilted mirror placed below samples. To establish the unique capabilities of MiSLFM, we performed extensive experiments, we observed various organelle interactions and intercellular interactions in different types of photosensitive cells under extremely low light conditions. Moreover, we demonstrated that superior axial resolution facilitates more robust blood cell tracking in zebrafish larvae at high speed.
Published. 2021, 10(12)
: 2380-2386
doi: 10.1038/s41377-021-00660-0
Color vision is used throughout medicine to interpret the health and status of tissue. Ionizing radiation used in radiation therapy produces broadband white light inside tissue through the Cherenkov effect, and this light is attenuated by tissue features as it leaves the body. In this study, a novel time-gated three-channel camera was developed for the first time and was used to image color Cherenkov emission coming from patients during treatment. The spectral content was interpreted by comparison with imaging calibrated tissue phantoms. Color shades of Cherenkov emission in radiotherapy can be used to interpret tissue blood volume, oxygen saturation and major vessels within the body.
Published. 2021, 10(12)
: 2387-2398
doi: 10.1038/s41377-021-00659-7
Inelastic quantum mechanical tunneling of electrons across plasmonic tunnel junctions can lead to surface plasmon polariton (SPP) and photon emission. So far, the optical properties of such junctions have been controlled by changing the shape, or the type of the material, of the electrodes, primarily with the aim to improve SPP or photon emission efficiencies. Here we show that by tuning the tunneling barrier itself, the efficiency of the inelastic tunneling rates can be improved by a factor of 3. We exploit the anisotropic nature of hexagonal boron nitride (hBN) as the tunneling barrier material in Au//hBN//graphene tunnel junctions where the Au electrode also serves as a plasmonic strip waveguide. As this junction constitutes an optically transparent hBN–graphene heterostructure on a glass substrate, it forms an open plasmonic system where the SPPs are directly coupled to the dedicated strip waveguide and photons outcouple to the far field. We experimentally and analytically show that the photon emission rate per tunneling electron is significantly improved (~ ×3) in Au//hBN//graphene tunnel junction due to the enhancement in the local density of optical states (LDOS) arising from the hBN anisotropy. With the dedicated strip waveguide, SPP outcoupling efficiency is quantified and is found to be ~80% stronger than the radiative outcoupling in Au//hBN//graphene due to the high LDOS of the SPP decay channel associated with the inelastic tunneling. The new insights elucidated here deepen our understanding of plasmonic tunnel junctions beyond the isotropic models with enhanced LDOS.
Published. 2021, 10(12)
: 2399-2407
doi: 10.1038/s41377-021-00671-x
Insightful knowledge on quantum nanostructured materials is paramount to engineer and exploit their vast gamut of applications. Here, a formalism based on the single-band effective mass equation was developed to determine the light absorption of colloidal quantum dots (CQDs) embedded in a wider bandgap semiconductor host, employing only three parameters (dots/host potential barrier, effective mass, and QD size). It was ascertained how to tune such parameters to design the energy level structure and consequent optical response. Our findings show that the CQD size has the biggest effect on the number and energy of the confined levels, while the potential barrier causes a linear shift of their values. While smaller QDs allow wider energetic separation between levels (as desired for most quantum-based technologies), the larger dots with higher number of levels are those that exhibit the strongest absorption. Nevertheless, it was unprecedently shown that such quantum-enabled absorption coefficients can reach the levels (104–105 cm−1) of bulk semiconductors.
Published. 2021, 10(12)
: 2408-2420
doi: 10.1038/s41377-021-00675-7
GeSn alloys are promising materials for CMOS-compatible mid-infrared lasers manufacturing. Indeed, Sn alloying and tensile strain can transform them into direct bandgap semiconductors. This growing laser technology however suffers from a number of limitations, such as poor optical confinement, lack of strain, thermal, and defects management, all of which are poorly discussed in the literature. Herein, a specific GeSn-on-insulator (GeSnOI) stack using stressor layers as dielectric optical claddings is demonstrated to be suitable for a monolithically integration of planar Group-Ⅳ semiconductor lasers on a versatile photonic platform for the near- and mid-infrared spectral range. Microdisk-shape resonators on mesa structures were fabricated from GeSnOI, after bonding a Ge0.9Sn0.1 alloy layer grown on a Ge strain-relaxed-buffer, itself on a Si(001) substrate. The GeSnOI microdisk mesas exhibited significantly improved optical gain as compared to that of conventional suspended microdisk resonators formed from the as-grown layer. We further show enhanced vertical out-coupling of the disk whispering gallery mode in-plane radiation, with up to 30% vertical out-coupling efficiency. As a result, the GeSnOI approach can be a valuable asset in the development of silicon-based mid-infrared photonics that combine integrated sources in a photonic platform with complex lightwave engineering.
Published. 2021, 10(12)
: 2421-2442
doi: 10.1038/s41377-021-00674-8
An invasive biopsy followed by histological staining is the benchmark for pathological diagnosis of skin tumors. The process is cumbersome and time-consuming, often leading to unnecessary biopsies and scars. Emerging noninvasive optical technologies such as reflectance confocal microscopy (RCM) can provide label-free, cellular-level resolution, in vivo images of skin without performing a biopsy. Although RCM is a useful diagnostic tool, it requires specialized training because the acquired images are grayscale, lack nuclear features, and are difficult to correlate with tissue pathology. Here, we present a deep learning-based framework that uses a convolutional neural network to rapidly transform in vivo RCM images of unstained skin into virtually-stained hematoxylin and eosin-like images with microscopic resolution, enabling visualization of the epidermis, dermal-epidermal junction, and superficial dermis layers. The network was trained under an adversarial learning scheme, which takes ex vivo RCM images of excised unstained/label-free tissue as inputs and uses the microscopic images of the same tissue labeled with acetic acid nuclear contrast staining as the ground truth. We show that this trained neural network can be used to rapidly perform virtual histology of in vivo, label-free RCM images of normal skin structure, basal cell carcinoma, and melanocytic nevi with pigmented melanocytes, demonstrating similar histological features to traditional histology from the same excised tissue. This application of deep learning-based virtual staining to noninvasive imaging technologies may permit more rapid diagnoses of malignant skin neoplasms and reduce invasive skin biopsies.
Published. 2021, 10(12)
: 2443-2454
doi: 10.1038/s41377-021-00677-5
Ratiometric luminescence thermometry with trivalent lanthanide ions and their 4fn energy levels is an emerging technique for non-invasive remote temperature sensing with high spatial and temporal resolution. Conventional ratiometric luminescence thermometry often relies on thermal coupling between two closely lying energy levels governed by Boltzmann's law. Despite its simplicity, Boltzmann thermometry with two excited levels allows precise temperature sensing, but only within a limited temperature range. While low temperatures slow down the nonradiative transitions required to generate a measurable population in the higher excitation level, temperatures that are too high favour equalized populations of the two excited levels, at the expense of low relative thermal sensitivity. In this work, we extend the concept of Boltzmann thermometry to more than two excited levels and provide quantitative guidelines that link the choice of energy gaps between multiple excited states to the performance in different temperature windows. By this approach, it is possible to retain the high relative sensitivity and precision of the temperature measurement over a wide temperature range within the same system. We demonstrate this concept using YAl3(BO3)4 (YAB): Pr3+, Gd3+ with an excited 6PJ crystal field and spin-orbit split levels of Gd3+ in the UV range to avoid a thermal black body background even at the highest temperatures. This phosphor is easily excitable with inexpensive and powerful blue LEDs at 450 nm. Zero-background luminescence thermometry is realized by using blue-to-UV energy transfer upconversion with the Pr3+−Gd3+ couple upon excitation in the visible range. This method allows us to cover a temperature window between 30 and 800 K.
Published. 2021, 10(12)
: 2455-2466
doi: 10.1038/s41377-021-00679-3
Collagen organization plays an important role in maintaining structural integrity and determining tissue function. Polarization-sensitive optical coherence tomography (PSOCT) is a promising noninvasive three-dimensional imaging tool for mapping collagen organization in vivo. While PSOCT systems with multiple polarization inputs have demonstrated the ability to visualize depth-resolved collagen organization, systems, which use a single input polarization state have not yet demonstrated sufficient reconstruction quality. Herein we describe a PSOCT based polarization state transmission model that reveals the depth-dependent polarization state evolution of light backscattered within a birefringent sample. Based on this model, we propose a polarization state tracing method that relies on a discrete differential geometric analysis of the evolution of the polarization state in depth along the Poincare sphere for depth-resolved birefringent imaging using only one single input polarization state. We demonstrate the ability of this method to visualize depth-resolved myocardial architecture in both healthy and infarcted rodent hearts (ex vivo) and collagen structures responsible for skin tension lines at various anatomical locations on the face of a healthy human volunteer (in vivo).
Published. 2021, 10(12)
: 2467-2481
doi: 10.1038/s41377-021-00676-6
The benchmark tin oxide (SnO2) electron transporting layers (ETLs) have enabled remarkable progress in planar perovskite solar cell (PSCs). However, the energy loss is still a challenge due to the lack of "hidden interface" control. We report a novel ligand-tailored ultrafine SnO2 quantum dots (QDs) via a facile rapid room temperature synthesis. Importantly, the ligand-tailored SnO2 QDs ETL with multi-functional terminal groups in situ refines the buried interfaces with both the perovskite and transparent electrode via enhanced interface binding and perovskite passivation. These novel ETLs induce synergistic effects of physical and chemical interfacial modulation and preferred perovskite crystallization-directing, delivering reduced interface defects, suppressed non-radiative recombination and elongated charge carrier lifetime. Power conversion efficiency (PCE) of 23.02% (0.04 cm2) and 21.6% (0.98 cm2, VOC loss: 0.336 V) have been achieved for the blade-coated PSCs (1.54 eV Eg) with our new ETLs, representing a record for SnO2 based blade-coated PSCs. Moreover, a substantially enhanced PCE (VOC) from 20.4% (1.15 V) to 22.8% (1.24 V, 90 mV higher VOC, 0.04 cm2 device) in the blade-coated 1.61 eV PSCs system, via replacing the benchmark commercial colloidal SnO2 with our new ETLs.
Published. 2021, 10(12)
: 2482-2491
doi: 10.1038/s41377-021-00678-4
Controlling the optical response of a medium through suitably tuned coherent electromagnetic fields is highly relevant in a number of potential applications, from all-optical modulators to optical storage devices. In particular, electromagnetically induced transparency (EIT) is an established phenomenon in which destructive quantum interference creates a transparency window over a narrow spectral range around an absorption line, which, in turn, allows to slow and ultimately stop light due to the anomalous refractive index dispersion. Here we report on the observation of a new form of both induced transparency and amplification of a weak probe beam in a strongly driven silicon photonic crystal resonator at room temperature. The effect is based on the oscillating temperature field induced in a nonlinear optical cavity, and it reproduces many of the key features of EIT while being independent of either atomic or mechanical resonances. Such thermo-optically induced transparency will allow a versatile implementation of EIT-analogs in an integrated photonic platform, at almost arbitrary wavelength of interest, room temperature and in a practical, low cost, and scalable system.
Published. 2021, 10(12)
: 2492-2506
doi: 10.1038/s41377-021-00682-8
Laser speckle contrast imaging (LSCI) is a powerful tool to monitor blood flow distribution and has been widely used in studies of microcirculation, both for animal and clinical applications. Conventionally, LSCI usually works on reflective-detected mode. However, it could provide promising temporal and spatial resolution for in vivo applications only with the assistance of various tissue windows, otherwise, the overlarge superficial static speckle would extremely limit its contrast and resolution. Here, we systematically investigated the capability of transmissive-detected LSCI (TR-LSCI) for blood flow monitoring in thick tissue. Using Monte Carlo simulation, we theoretically compared the performance of transmissive and reflective detection. It was found that the reflective-detected mode was better when the target layer was at the very surface, but the imaging quality would rapidly decrease with imaging depth, while the transmissive-detected mode could obtain a much stronger signal-to-background ratio (SBR) for thick tissue. We further proved by tissue phantom, animal, and human experiments that in a certain thickness of tissue, TR-LSCI showed remarkably better performance for thick-tissue imaging, and the imaging quality would be further improved if the use of longer wavelengths of near-infrared light. Therefore, both theoretical and experimental results demonstrate that TR-LSCI is capable of obtaining thick-tissue blood flow information and holds great potential in the field of microcirculation research.
Published. 2021, 10(12)
: 2507-2517
doi: 10.1038/s41377-021-00687-3
Using a single biological element as a photonic component with well-defined features has become a new intriguing paradigm in biophotonics. Here we show that endogenous lipid droplets in the mature adipose cells can behave as fully biocompatible microlenses to strengthen the ability of microscopic imaging as well as detecting intra- and extracellular signals. By the assistance of biolenses made of the lipid droplets, enhanced fluorescence imaging of cytoskeleton, lysosomes, and adenoviruses has been achieved. At the same time, we demonstrated that the required excitation power can be reduced by up to 73%. The lipidic microlenses are finely manipulated by optical tweezers in order to address targets and perform their real-time imaging inside the cells. An efficient detecting of fluorescence signal of cancer cells in extracellular fluid was accomplished due to the focusing effect of incident light by the lipid droplets. The lipid droplets acting as endogenous intracellular microlenses open the intriguing route for a multifunctional biocompatible optics tool for biosensing, endoscopic imaging, and single-cell diagnosis.
Published. 2021, 10(12)
: 2518-2530
doi: 10.1038/s41377-021-00681-9
The ability to quantify optical properties (i.e., absorption and scattering) of strongly turbid media has major implications on the characterization of biological tissues, fluid fields, and many others. However, there are few methods that can provide wide-field quantification of optical properties, and none is able to perform quantitative optical property imaging with high-speed (e.g., kilohertz) capabilities. Here we develop a new imaging modality termed halftone spatial frequency domain imaging (halftone-SFDI), which is approximately two orders of magnitude faster than the state-of-the-art, and provides kilohertz high-speed, label-free, non-contact, wide-field quantification for the optical properties of strongly turbid media. This method utilizes halftone binary patterned illumination to target the spatial frequency response of turbid media, which is then mapped to optical properties using model-based analysis. We validate the halftone-SFDI on an array of phantoms with a wide range of optical properties as well as in vivo human tissue. We demonstrate with an in vivo rat brain cortex imaging study, and show that halftone-SFDI can longitudinally monitor the absolute concentration as well as spatial distribution of functional chromophores in tissue. We also show that halftone-SFDI can spatially map dual-wavelength optical properties of a highly dynamic flow field at kilohertz speed. Together, these results highlight the potential of halftone-SFDI to enable new capabilities in fundamental research and translational studies including brain science and fluid dynamics.
Published. 2021, 10(12)
: 2531-2540
doi: 10.1038/s41377-021-00685-5
The exploitation of ultrafast electron dynamics in quantum cascade lasers (QCLs) holds enormous potential for intense, compact mode-locked terahertz (THz) sources, squeezed THz light, frequency mixers, and comb-based metrology systems. Yet the important sub-cycle dynamics have been notoriously difficult to access in operational THz QCLs. Here, we employ high-field THz pulses to perform the first ultrafast two-dimensional spectroscopy of a free-running THz QCL. Strong incoherent and coherent nonlinearities up to eight-wave mixing are detected below and above the laser threshold. These data not only reveal extremely short gain recovery times of 2 ps at the laser threshold, they also reflect the nonlinear polarization dynamics of the QCL laser transition for the first time, where we quantify the corresponding dephasing times between 0.9 and 1.5 ps with increasing bias currents. A density-matrix approach reproducing the emergence of all nonlinearities and their ultrafast evolution, simultaneously, allows us to map the coherently induced trajectory of the Bloch vector. The observed high-order multi-wave mixing nonlinearities benefit from resonant enhancement in the absence of absorption losses and bear potential for a number of future applications, ranging from efficient intracavity frequency conversion, mode proliferation to passive mode locking.
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