Search for: All records

Non-degenerate two-photon absorption (NTA) offers an attractive route for wide-field mid-infrared imaging by mapping long wavelength information into the spectral detection windows of mature near-infrared detector technologies. However, existing NTA implementations rely almost exclusively on complex, large-footprint femtosecond laser systems, severely limiting practicality and scalability. Here, we demonstrate an NTA imaging platform that replaces the ultrafast laser with a compact nanosecond mid-IR source coupled to a high-definition indium gallium arsenide camera. Operating in the nanosecond regime removes stringent temporal-overlap requirements, dramatically simplifying system architecture while preserving high detection sensitivity. Using this approach, we achieve chemically selective, wide-field imaging deep into the mid-IR molecular fingerprint region and demonstrate, for the first time, video-rate NTA imaging in this spectrally rich regime. By combining relaxed alignment constraints, compact excitation, and high-speed fingerprint-region imaging, this work establishes nanosecond NTA as a practical and scalable foundation for next-generation mid-IR chemical imaging. 

Silicon’s indirect band gap severely suppresses radiative recombination, limiting its use as an efficient light-emitting material. Although nanoscale confinement of carriers, dielectric resonators, or plasmonic structures can partially mitigate this limitation, these approaches typically require complex fabrication. Here, we report a fundamentally different and scalable mechanism that enables efficient light emission directly from bulk silicon. By decorating a silicon wafer with ultrasmall (<2 nm) gold or copper particles, we observe intense luminescence spanning the visible and near-infrared. Remarkably, the emission is indistinguishable for Au and Cu decorations in both spectral and temporal domains, demonstrating that the confinement extent, not the material composition, governs the effect. We attribute the emission to spatially confined photonic states with broadened momentum distributions, enabling phonon-independent optical transitions otherwise forbidden in silicon. This mechanism yields quantum efficiencies comparable to those of direct-band-gap semiconductors and produces ∼a 10^5-fold enhancement in the integrated emission intensity, establishing a practical route toward silicon light-emitting devices. 

Collagen Types I and II share highly conserved triple‐helical backbones and similar C-H stretch vibrational spectra, which limits the ability of conventional spectroscopic or second‐harmonic generation methods to unambiguously distinguish between them in native and engineered matrices. By combining polarization‐resolved sum‐frequency generation (SFG) measurements with tensor‐based simulations of the C-H stretch response, this work identifies collagen's asymmetric mode measured via the XXY tensor element as a robust optical marker that exhibits distinct spatial symmetries for collagen Type I and Type II. In rat auricular cartilage, analysis of the polarization‐resolved SFG signatures combined with vertex component analysis reveals pocket‐like domains of differently oriented collagen Type II fibrils rather than a uniformly aligned network. These findings establish polarization‐resolved SFG microscopy as a structurally specific tool for mapping collagen Type II architecture and label‐free discrimination of collagen Types I and II. 

Nonlinear optical (NLO) imaging platforms traditionally rely on refractive microscope objectives, which suffer from chromatic aberrations and temporal dispersion of pulsed excitation light. These issues degrade spatial imaging properties and signal brightness. Furthermore, the limited transmission range of refractive materials restricts NLO imaging, especially for applications requiring short- to mid-wave infrared excitation. While reflective microscope objectives offer an achromatic solution and broader transmission range (from visible to mid-infrared), conventional Schwarzschild designs have a central obscuration, which limits transmission throughput, imparts diffraction effects into the images, and, more generally, hinders the adoption of reflective optics in NLO microscopy. We overcome these obscuration-based limitations by developing a reflective microscope objective using freeform mirrors in a non-coaxial geometry. This obscuration-free design boasts a 0.65 numerical aperture (NA), near diffraction-limited imaging performance, and offers significantly improved transmission with wider fields-of-view. We demonstrate its utility by integrating it into a standard laser-scanning microscope and performing NLO microscopy across a wide range of excitation wavelengths. Our freeform microscope objective outperforms standard reflective designs, providing an achromatic, dispersion-free alternative to refractive lenses for NLO imaging. 

The development and application of nonlinear optical (NLO) microscopy methods in biomedical research has experienced rapid growth over the past three decades. Despite the compelling power of these methods, optical scattering limits their practical use in biological tissues. This tutorial offers a model-based approach illustrating how analytical methods from classical electromagnetism can be employed to comprehensively model NLO microscopy in scattering media. In Part I, we quantitatively model focused beam propagation in non-scattering and scattering media from the lens to focal volume. In Part II, we model signal generation, radiation, and far-field detection. Moreover, we detail modeling approaches for major optical microscopy modalities including classical fluorescence, multi-photon fluorescence, second harmonic generation, and coherent anti-Stokes Raman microscopy. 

The development and application of nonlinear optical (NLO) microscopy methods in biomedical research have experienced rapid growth over the past three decades. Despite the compelling power of these methods, optical scattering limits their practical use in biological tissues. This tutorial offers a model-based approach illustrating how analytical methods from classical electromagnetism can be employed to comprehensively model NLO microscopy in scattering media. In Part I, we quantitatively model focused beam propagation in non-scattering and scattering media from the lens to focal volume. In Part II, we model signal generation, radiation, and far-field detection. Moreover, we detail modeling approaches for major optical microscopy modalities including classical fluorescence, multi-photon fluorescence, second harmonic generation, and coherent anti-Stokes Raman microscopy. 

We theoretically show that the optical chiral properties of tightly focused laser beams can be characterized by means of force detection. To measure the chiral properties of a beam of given handedness in the microscopic focal volume, we determine the photoinduced force exerted on a sharp tip, which is illuminated first by the beam of interest and second by an auxiliary beam of opposite handedness, in a sequential manner. We show that the difference between the force measurements is directly proportional to the chiral properties of the beam of interest. In particular, the gradient force difference Δ⟨Fgrad ,z⟩ is found to have exclusive correspondence to the time-averaged helicity density of the incident light, whereas the differential scattering force provides information about the spin angular momentum density of light. We further characterize and quantify the helicity-dependent Δ⟨Fgrad ,z⟩ using a Mie scattering formalism complemented with full wave simulations, underlining that the magnitude of the difference force is within an experimentally detectable range. 

Photo-induced force microscopy (PiFM) is a scan probe technique that offers images with spectroscopic contrast at a spatial resolution in the nanometer range. PiFM utilizes the non-propagating, enhanced near field at the apex of a sharp tip to locally induce a polarization in the sample, which in turn produces an additional force acting on the cantilevered tip. This photo-induced force, though in the pN range or less, can be extracted from the oscillation properties of the cantilever, thus enabling the generation of photo-induced force maps. Since its inception in 2010, the PiFM technique has grown into a useful nano-spectrocopic tool that has expanded its reach in terms of imaging capabilities and applications. In this review, we present various technical implementations of the PiFM approach. In addition, we discuss the physical origin of the PiFM signal, highlighting the contributions from dipole–dipole forces as well as forces that derive from photo-thermal processes.