Spectroscopic Information Research Articles

Multispectral Microscopic Multiplexed (3M) Imaging of Atomically‐Thin Crystals Using Deep Learning

AbstractUltra‐thin atomic crystals are promising for fabricating next‐generation photonic and optoelectronic devices. Wafer‐scale characterization techniques are highly desired for efficient and accurate thickness identification of these crystals and their heterostructures. Optical contrast between atomic crystals and substrates based on Fresnel theory is a key technique for the identification of thicknesses. Both RGB color information and spectroscopic information have been explored for layer number counting and implemented with machine learning algorithms based on large amounts of data for feature extraction. In this work, a multispectral microscopic method combining the hardware design and deep‐learning algorithms is developed. Multispectral image restoration during large‐area scanning caused by optical imaging modality drifts and automated layer number identification based on multispectral grayscale images are studied using deep learning models: generative adversarial network (GAN) and 3D U‐Net. These models are trained using custom‐built multispectral data sets and evaluated quantitatively with indicators (Dice coefficient, confusion matrix, structural similarity). After these models are trained and tested, they are integrated into a graphic user interface for on‐site identification use. The developed method provides a framework using multispectral images for 3D data reconstruction and segmentation and can be implemented for wafer‐scale characterization of heterostructures containing different species of ultra‐thin atomic crystals.

Ultra wideband NIR emission in all-inorganic lead-free metal halides through Sb3+ doping

In recent years, food detection, plant photosynthesis, night vision, and the identification of biological data have all benefited from near-infrared luminescence. However, developing metal halides emitting near-infrared (NIR) light is still difficult, which restricts further applicability. Here, we propose an insightful methodology to investigate the wideband NIR emission in metal halide Cs2ZnCl4 host by doping Sb3+. The phosphors are successfully synthesized by the coprecipitation method and the photoluminescent properties are explored in detail. Based on the spectroscopic information, experimental data with DFT calculations, and luminescence kinetics investigation of Sb3+ doped Cs2ZnCl4, the broadband red emission is caused by self-trapped excitons, which can be attributed to the 3P1–1S0 transitions. The spectra under the excitation at 351 nm exhibit an ultra-wideband emission with a center wavelength of 737 nm, an FHWM of 196 nm, and a significant Stokes shift of 386 nm. The NIR LED fabricated by Cs2ZnCl4: Sb3+ can also be used in night vision devices and biological identification. Our findings in Sb3+ doped Cs2ZnCl4 materials provide light on how doping induces emission centers and expand our understanding of the optical characteristics of doped lead-free metal halides for future research. This work also offers recommendations for broadening the range of uses for luminous metal halides and proposes an efficient method for developing fresh environmentally friendly and wideband emission NIR phosphors.

Development of PCA-MLP Model Based on Visible and Shortwave Near Infrared Spectroscopy for Authenticating Arabica Coffee Origins.

Arabica coffee, one of Indonesia's economically important coffee commodities, is commonly subject to fraud due to mislabeling and adulteration. In many studies, spectroscopic techniques combined with chemometric methods have been massively employed in classification issues, such as principal component analysis (PCA) and discriminant analyses, compared to machine learning models. In this study, spectroscopy combined with PCA and a machine learning algorithm (artificial neural network, ANN) were developed to verify the authenticity of Arabica coffee collected from four geographical origins in Indonesia, including Temanggung, Toraja, Gayo, and Kintamani. Spectra from pure green coffee were collected from Vis-NIR and SWNIR spectrometers. Several preprocessing techniques were also applied to attain precise information from spectroscopic data. First, PCA compressed spectroscopic information and generated new variables called PCs scores, which would become inputs for the ANN model. The discrimination of Arabica coffee from different origins was conducted with a multilayer perceptron (MLP)-based ANN model. The accuracy attained ranged from 90% to 100% in the internal cross-validation, training, and testing sets. The error in the classification process did not exceed 10%. The generalization ability of the MLP combined with PCA was superior, suitable, and successful for verifying the origin of Arabica coffee.

Thickness Mapping and Layer Number Identification of Exfoliated van der Waals Materials by Fourier Imaging Micro-Ellipsometry

As performance of van der Waals heterostructure devices is governed by the nanoscale thicknesses and homogeneity of their constituent mono- to few-layer flakes, accurate mapping of these properties with high lateral resolution becomes imperative. Spectroscopic ellipsometry is a promising optical technique for such atomically thin-film characterization due to its simplicity, noninvasive nature and high accuracy. However, the effective use of standard ellipsometry methods on exfoliated micron-scale flakes is inhibited by their tens-of-microns lateral resolution or slow data acquisition. In this work, we demonstrate a Fourier imaging spectroscopic micro-ellipsometry method with sub-5 μm lateral resolution and three orders-of-magnitude faster data acquisition than similar-resolution ellipsometers. Simultaneous recording of spectroscopic ellipsometry information at multiple angles results in a highly sensitive system, which is used for performing angstrom-level accurate and consistent thickness mapping on exfoliated mono-, bi- and trilayers of graphene, hexagonal boron nitride (hBN) and transition metal dichalcogenide (MoS2, WS2, MoSe2, WSe2) flakes. The system can successfully identify highly transparent monolayer hBN, a challenging proposition for other characterization tools. The optical microscope integrated ellipsometer can also map minute thickness variations over a micron-scale flake, revealing its lateral inhomogeneity. The prospect of adding standard optical elements to augment generic optical imaging and spectroscopy setups with accurate in situ ellipsometric mapping capability presents potential opportunities for investigation of exfoliated 2D materials.

The odd bunch: chrono-chemo-dynamics of sixteen unusual stars from Kepler

ABSTRACT In this study we combine asteroseismic, spectroscopic, and kinematic information to perform a detailed analysis of a sample of 16 stars from the Kepler field. Our selection focuses on stars that appear to contradict Galactic chemical evolution models: young and α-rich, old and metal-rich, as well as other targets with unclear classification in past surveys. Kinematics are derived from Gaia DR3 parallaxes and proper motions, and high-resolution spectra from HIRES/Keck are used to calculate chemical abundances for over 20 elements. This information is used to perform careful checks on asteroseismic masses and ages derived via grid-based modelling. Among the seven stars previously classified as young and α-rich, only one seems to be an unambiguously older object masking its true age. We confirm the existence of two very old (≥11 Gyr), super metal-rich (≥0.1 dex) giants. These two stars have regular thin disc chemistry and in-plane solar circle orbits that fit well in the picture of radial migration via the churning mechanism. The alternative explanation that these stars have younger ages would require mass-loss rates that strongly increase with increasing metallicity. Finally, we suggest further investigations to explore the suitability of Zn as a chemical clock in red giants.

Gamma spectroscopy of even-even Ytterbium isotopes

The even-even Ytterbium isotopes lack spectroscopic information with the increase of the neutron number and they are well deformed nuclei, presenting rotational properties. In this mass region of the nuclear chart predictions have shown rare phenomena related to nuclear structure, such as shape coexistence. In this work the population of excited states were investigated in the even-even Yb isotopes via the 2n-transfer reaction 168-174Yb (18O, 16O) 170-176Yb. The measurements were carried out at the 9 MV Tandem accelerator at the Horia Hulubei National Institute of Physics and Nuclear Engineering (IFIN-HH) in Romania. The deduced gamma-ray angular distributions in the ground state bands are found to correspond with transitions, as expected

Microsphere‐Aided Super‐Resolution Scanning Spectral and Photocurrent Microscopy for Optoelectronic Devices

AbstractDielectric microspheres naturally possess unique optical properties by which the light's focus and confinement can be manipulated on a microscale. Combining microspheres and optical or Raman microscopy, super‐resolution imaging beyond the diffraction limit and enhancement of Raman signals are demonstrated to provide abundant spectroscopic information on materials. However, microsphere‐aided super‐resolution scanning photocurrent imaging remains challenging to date. Here, based on the photonic nanojet mechanism, a super‐resolution photocurrent and spectral microscopy equipped with a scanning tip with silica dielectric microspheres are presented. With such microsphere‐aided microscopy, order of magnitude enhancements for single‐point Raman and photoluminescence signals can be achieved, and the spatial resolutions for photocurrent and spectral mapping surpass the best resolution of the original confocal system restricted by the diffraction limit. This versatile system enables correlative super‐resolution spectral and photocurrent imaging, serving as a reliable tool for comprehensively understanding and uncovering the optoelectronic properties of materials.

Proton decays from α -unbound states in Mg22 and the Ne18(α,p0)21Na cross section

Background: Type I x-ray bursts provide an opportunity to constrain the equation of state of nuclear matter. Observations of the light curves from these bursts allow the compactness of neutron stars to be constrained. However, the behavior of these light curves also depends on a number of important thermonuclear reaction rates. One of these reactions, $^{18}\mathrm{Ne}(\ensuremath{\alpha},p)^{21}\mathrm{Na}$, has been extensively studied but there is some tension between the rate calculated from spectroscopic information of states above the $\ensuremath{\alpha}$-particle threshold in $^{22}\mathrm{Mg}$ and the rate determined from time-reversed measurements of the cross section.Purpose: The time-reversed measurement of the cross section is only sensitive to the ground state-to-ground state contribution. Therefore, corrections must be made to this reaction rate to account for the contribution of branches to excited states in $^{21}\mathrm{Na}$. At present this is done with statistical models which may not be applicable in such light nuclei. Basing the correction of the time-reversed cross section on experimental data is much more robust.Method: The $^{24}\mathrm{Mg}(p,t)^{22}\mathrm{Mg}$ reaction was used to populate states in $^{22}\mathrm{Mg}$. The reaction products from the reaction were analysed by the K600 magnetic spectrometer at iThemba Laboratories, South Africa. Protons decaying from excited states of $^{22}\mathrm{Mg}$ (${S}_{p}=5502$ keV) were detected in an array of five double-sided silicon strip detectors placed at backward angles. The branching ratio for proton decays to the ground state of $^{21}\mathrm{Na}, {B}_{{p}_{0}}$, was determined by comparing the inclusive (triton-only focal-plane) and exclusive (focal-plane gated on a specific proton decay) spectra.Results: The experimental proton decay branching ratio to the ground state of $^{21}\mathrm{Na}$ from excited states in $^{22}\mathrm{Mg}$ were found to be a factor of about two smaller than the ratios predicted by Hauser-Feshbach models. Using the experimental branchings for a recalculation of the $^{18}\mathrm{Ne}(\ensuremath{\alpha},{p}_{0})^{21}\mathrm{Na}$ cross section leads to a considerably improved agreement with previous reaction data. Updated information on the disputed number of levels around ${E}_{x}\ensuremath{\approx}9$ MeV and on the possible $^{18}\mathrm{Ne}(\ensuremath{\alpha},2p)^{20}\mathrm{Ne}$ cross section at astrophysical energies is also reported.Conclusions: The proton decay branching of excited states in $^{22}\mathrm{Mg}$ to the ground state of $^{21}\mathrm{Na}$ have been measured using the K600 Q2D spectrometer at iThemba Laboratories coupled to the double-sided silicon-strip detector array CAKE. Using these experimental data, the modeling of the $^{18}\mathrm{Ne}(\ensuremath{\alpha},{p}_{0})^{21}\mathrm{Na}$ cross section has been improved. The result is not only in better agreement with previous cross section data but also consistent with a recent direct measurement of $^{18}\mathrm{Ne}(\ensuremath{\alpha},p)^{21}\mathrm{Na}$. This strengthens the case for the application of statistical models for these reactions.

CN and CO features: key indicators of red giant evolutionary phase in moderate-resolution X-shooter spectra

ABSTRACT Data-driven analysis methods can help to infer physical properties of red giant stars where ‘gold-standard’ asteroseismic data are not available. The study of optical and infrared spectra of red giant stars with data-driven analyses has revealed that differences in oscillation frequencies and their separations are imprinted in said spectra. This makes it possible to confidently differentiate core helium burning red clump (RC) stars from those that are still on their first ascent of the red giant branch (RGB). We extend these studies to a tenfold larger wavelength range of 0.33–2.5 µm with the moderate-resolution VLT/X-shooter spectrograph. Our analysis of 49 stars with asteroseismic data from the K2 mission confirms that CN, CO, and CH features are indeed the primary carriers of spectroscopic information on the evolutionary stages of red giant stars. We report 215 informative features for differentiating the RC from the RGB within the range of 0.33–2.5 µm. This makes it possible for existing and future spectroscopic surveys to optimize their wavelength regions to deliver both a large variety of elemental abundances and reliable age estimates of luminous red giant stars.

Probing the graphene/substrate interaction by electron tunneling decay

The electronic properties of graphene can be modified by the local interaction with a selected metal substrate. To probe this effect, Scanning Tunneling Microscopy is widely employed, particularly by means of local measurement via lock-in amplifier of the differential conductance and of the field emission resonance. In this article we propose an alternative, reliable method of probing the graphene/substrate interaction that is readily available to any STM apparatus. By testing the tunneling current as function of the tip/sample distance on nanostructured graphene on Ni(100) and Ir (100), we demonstrate that I(z) spectroscopy can be quantitatively compared with Density Functional Theory calculations and can be used to assess the nature of the interaction between graphene and substrate. This method can expand the capabilities of standard STM systems to study graphene/substrate complexes, complementing standard topographic probing with spectroscopic information.

Advancing Spectrally-Resolved Single Molecule Localization Microscopy with Deep Learning.

Spectrally-resolved single molecule localization microscopy (srSMLM) is a recent technique enriching single molecule localization microscopy with the simultaneous recording of spectra of the single emitters. srSMLM resolution is limited by the number of photons collected per emitters. Sharing a photon budget to record the localization and the spectroscopic information results in a loss of spatial and spectral resolution-or forces the sacrifice of one at the expense of the other. Here, srUnet-a deep-learning Unet-based image processing routine trained to increase the spectral and spatial signals to compensate for the resolution loss inherent in additionally recording the spectral component is reported. Both localization and spectral precision are improved by srUnet-particularly for the low-emitting species. srUnet increases the fraction of localization whose signal can be both spatially and spectrally characterized. It preserves spectral shifts and the linearity of the dispersion of light. It strongly facilitates wavelength assignment in multicolor experiments. srUnet is a simple post-processing add-on boosting srSMLM performance close to conventional SMLM with the potential to turn srSMLM into the new standard for multicolor single molecule imaging.

Three cases of optical periodic modulation in Active Galactic Nuclei

ABSTRACT We report on the case of optical periodic modulation discovered in two Active Galactic Nuclei (AGN) and one candidate AGN. Analysing the archival optical data obtained from large transient surveys, namely the Catalina Real-Transient Survey (CRTS) and the Zwicky Transient Facility (ZTF), we find periodicities of 2169.7, 2103.1, and 1462.6 d in sources J0122 + 1032, J1007 + 1248 (or PG 1004 + 1248), and J2131 − 1127, respectively. The optical spectra of the first two indicate that the first is likely a blazar and the second a type 1 Seyfert galaxy, and while no spectroscopic information is available for the third one, its overall properties suggest that it is likely an AGN. In addition, mid-infrared (MIR) light-curve data of the three sources, taken by the Wide-field Infrared Survey Explorer (WISE), are also analysed. The light curves show significant variations, but not appearing related to the optical periodicities. Based on the widely discussed supermassive black hole binary (SMBHB) scenario, we discuss the origin of the optical modulation. Two possible interesting features, an additional 162-d short optical periodicity in J2131 − 1127 and the consistency of the X-ray flux variations of J1007 + 1248 with its optical periodicity, are also discussed within the SMBHB scenario.

Near-field terahertz nonlinear optics with blue light

The coupling of terahertz optical techniques to scattering-type scanning near-field microscopy (s-SNOM) has recently emerged as a valuable new paradigm for probing the properties of semiconductors and other materials on the nanoscale. Researchers have demonstrated a family of related techniques, including terahertz nanoscopy (elastic scattering, based on linear optics), time-resolved methods, and nanoscale terahertz emission spectroscopy. However, as with nearly all examples of s-SNOM since the technique’s inception in the mid-1990s, the wavelength of the optical source coupled to the near-field tip is long, usually at energies of 2.5 eV or less. Challenges in coupling of shorter wavelengths (i.e., blue light) to the nanotip has greatly inhibited the study of nanoscale phenomena in wide bandgap materials such as Si and GaN. Here, we describe the first experimental demonstration of s-SNOM using blue light. With femtosecond pulses at 410 nm, we generate terahertz pulses directly from bulk silicon, spatially resolved with nanoscale resolution, and show that these signals provide spectroscopic information that cannot be obtained using near-infrared excitation. We develop a new theoretical framework to account for this nonlinear interaction, which enables accurate extraction of material parameters. This work establishes a new realm of possibilities for the study of technologically relevant wide-bandgap materials using s-SNOM methods.

Imaging-based intelligent spectrometer on a plasmonic rainbow chip

Compact, lightweight, and on-chip spectrometers are required to develop portable and handheld sensing and analysis applications. However, the performance of these miniaturized systems is usually much lower than their benchtop laboratory counterparts due to oversimplified optical architectures. Here, we develop a compact plasmonic “rainbow” chip for rapid, accurate dual-functional spectroscopic sensing that can surpass conventional portable spectrometers under selected conditions. The nanostructure consists of one-dimensional or two-dimensional graded metallic gratings. By using a single image obtained by an ordinary camera, this compact system can accurately and precisely determine the spectroscopic and polarimetric information of the illumination spectrum. Assisted by suitably trained deep learning algorithms, we demonstrate the characterization of optical rotatory dispersion of glucose solutions at two-peak and three-peak narrowband illumination across the visible spectrum using just a single image. This system holds the potential for integration with smartphones and lab-on-a-chip systems to develop applications for in situ analysis.

Evolutionary and Observational Properties of Red Giant Acoustic Glitch Signatures

While solar-like oscillations in red giants have been observed at massive scales by the Kepler mission, few features of these oscillation mode frequencies, other than their global properties, have been exploited for stellar characterization. The signatures of acoustic glitches in mode frequencies have been used for studying main-sequence stars, but the validity of applying such techniques to evolved red giants, particularly pertaining to the inclusion of nonradial modes, has been less well examined. Making use of new theoretical developments, we characterize glitches using the π modes associated with red giant stellar models, and use our procedure to examine for the first time how the properties of the He ii acoustic glitch—specifically its amplitude and associated acoustic depth—vary over the course of evolution up the red giant branch, and with respect to other fundamental stellar properties. We find that the acoustic depths of these glitches, in conjunction with other spectroscopic information, discriminate between red giants in the first-ascent and core-helium-burning phases. We critically reexamine previous attempts to constrain acoustic glitches from nonradial (in particular dipole) modes in red giants. Finally, we apply our fitting procedure to Kepler data, to evaluate its robustness to noise and other observational systematics.

WEAVE-StePS: A stellar population survey using WEAVE at WHT

Context. The upcoming new generation of optical spectrographs on four-meter-class telescopes will provide valuable opportunities for forthcoming galaxy surveys through their huge multiplexing capabilities, excellent spectral resolution, and unprecedented wavelength coverage. Aims. WEAVE is a new wide-field spectroscopic facility mounted on the 4.2 m William Herschel Telescope in La Palma. WEAVE-StePS is one of the five extragalactic surveys that will use WEAVE during its first five years of operations. It will observe galaxies using WEAVE MOS (∼950 fibres distributed across a field of view of ∼3 square degrees on the sky) in low-resolution mode (R ∼ 5000, spanning the wavelength range 3660 − 9590 Å). Methods. WEAVE-StePS will obtain high-quality spectra (S/N ∼ 10 Å−1 at R ∼ 5000) for a magnitude-limited (IAB = 20.5) sample of ∼25 000 galaxies, the majority selected at z ≥ 0.3. The survey goal is to provide precise spectral measurements in the crucial interval that bridges the gap between LEGA-C and SDSS data. The wide area coverage of ∼25 square degrees will enable us to observe galaxies in a variety of environments. The ancillary data available in each of the observed fields (including X-ray coverage, multi-narrow-band photometry and spectroscopic redshift information) will provide an environmental characterisation for each observed galaxy. Results. This paper presents the science case of WEAVE-StePS, the fields to be observed, the parent catalogues used to define the target sample, and the observing strategy that was chosen after a forecast of the expected performance of the instrument for our typical targets. Conclusions. WEAVE-StePS will go back further in cosmic time than SDSS, extending its reach to encompass more than ∼6 Gyr. This is nearly half of the age of the Universe. The spectral and redshift range covered by WEAVE-StePS will open a new observational window by continuously tracing the evolutionary path of galaxies in the largely unexplored intermediate-redshift range.

Phase-space Properties and Chemistry of the Sagittarius Stellar Stream Down to the Extremely Metal-poor ([Fe/H] ≲ −3) Regime

In this work, we study the phase-space and chemical properties of the Sagittarius (Sgr) stream, the tidal tails produced by the ongoing destruction of the Sgr dwarf spheroidal (dSph) galaxy, focusing on its very metal-poor (VMP; [Fe/H] < −2) content. We combine spectroscopic and astrometric information from SEGUE and Gaia EDR3, respectively, with data products from a new large-scale run of the StarHorse spectrophotometric code. Our selection criteria yield ∼1600 stream members, including >200 VMP stars. We find the leading arm (b > 0°) of the Sgr stream to be more metal-poor, by ∼0.2 dex, than the trailing one (b < 0°). With a subsample of turnoff and subgiant stars, we estimate this substructure’s stellar population to be ∼1 Gyr older than the thick disk’s. With the aid of an N-body model of the Sgr system, we verify that simulated particles stripped earlier (>2 Gyr ago) have present-day phase-space properties similar to lower metallicity stream stars. Conversely, those stripped more recently (<2 Gyr) are preferentially akin to metal-rich ([Fe/H] > −1) members of the stream. Such correlation between kinematics and chemistry can be explained by the existence of a dynamically hotter, less centrally concentrated, and more metal-poor population in Sgr dSph prior to its disruption, implying that this galaxy was able to develop a metallicity gradient before its accretion. Finally, we identified several carbon-enhanced metal-poor ([C/Fe] > +0.7 and [Fe/H] ≤ −1.5) stars in the Sgr stream, which might be in tension with current observations of its remaining core where such objects are not found.

Lyman continuum leaker candidates among highly ionised, low-redshift dwarf galaxies selected from He II

Context. Contemporary research suggests that the reionisation of the intergalactic medium (IGM) in the early Universe was predominantly realised by star-forming (proto-)galaxies (SFGs). Due to observational constraints, our knowledge on the origins of sufficient amounts of ionising Lyman continuum (LyC) photons and the mechanisms facilitating their transport into the IGM remains sparse. Recent efforts have thus focussed on the study of local analogues to these high-redshift objects. Aims. We aim to acquire a set of very low-redshift SFGs that exhibit signs of a hard radiation field being present. A subsequent analysis of their emission line properties is intended to shed light on how the conditions prevalent in these objects compare to those predicted to be present in early SFGs that are thought to be LyC emitters (LCEs). Methods. We used archival spectroscopic SDSS DR12 data to select a sample of low-redshift He II 4686 emitters and restricted it to a set of SFGs with an emission line diagnostic sensitive to the presence of an active galactic nucleus, which serves as our only selection criterion. We performed a population spectral synthesis with FADO to reconstruct these galaxies’ star-formation histories (SFHs). Utilising the spectroscopic information at hand, we constrained the predominant ionisation mechanisms in these galaxies and inferred information on interstellar medium (ISM) conditions relevant for the escape of LyC radiation. Results. Our final sample consists of eighteen ionised, metal-poor galaxies (IMPs). These low-mass (6.2 ≤ log(M⋆/M⊙) ≤ 8.8), low-metallicity (7.54 ≤ log(O/H) + 12 ≤ 8.13) dwarf galaxies appear to be predominantly ionised by stellar sources. We find large [OIII] 5007/[OII] 3727 ratios and [SII] 6717,6731/Hα deficiencies, which provide strong indications for these galaxies to be LCEs. At least 40% of these objects are candidates for featuring cosmologically significant LyC escape fractions ≳10%. The IMPs’ SFHs exhibit strong similarities and almost all galaxies appear to contain an old (&gt; 1 Gyr) stellar component, while also harbouring a young, two-stage (∼10 Myr and &lt; 1 Myr) starburst, which we speculate might be related to LyC escape. Conclusions. The properties of the compact emission line galaxies presented here align well with those observed in many local LCEs. In fact, our sample may prove as an extension to the rather small catalogue of local LCEs, as the extreme ISM conditions we find are assumed to facilitate LyC leakage. Notably, all of our eighteen candidates are significantly closer (z &lt; 0.1) than most established LCEs. If the inferred LyC photon loss is genuine, this demonstrates that selecting SFGs from He II 4686 is a powerful selection criterion in the search for LCEs.

3D Chemical Imaging by Fluorescence-detected Mid-Infrared Photothermal Fourier Light Field Microscopy.

Three-dimensional molecular imaging of living organisms and cells plays a significant role in modern biology. Yet, current volumetric imaging modalities are largely fluorescence-based and thus lack chemical content information. Mid-infrared photothermal microscopy as a chemical imaging technology provides infrared spectroscopic information at submicrometer spatial resolution. Here, by harnessing thermosensitive fluorescent dyes to sense the mid-infrared photothermal effect, we demonstrate 3D fluorescence-detected mid-infrared photothermal Fourier light field (FMIP-FLF) microscopy at the speed of 8 volumes per second and submicron spatial resolution. Protein contents in bacteria and lipid droplets in living pancreatic cancer cells are visualized. Altered lipid metabolism in drug-resistant pancreatic cancer cells is observed with the FMIP-FLF microscope.

Distinguishing Single-Metal Nanoparticles with Subdiffraction Spatial Resolution Using Variable-Polarization Fourier Transform Nonlinear Optical Microscopy.

The development and use of interferometric variable-polarization Fourier transform nonlinear optical (vpFT-NLO) imaging to distinguish colloidal nanoparticles colocated within the optical diffraction limit is described. Using a collinear train of phase-stabilized pulse pairs with orthogonal electric field vectors, the polarization of nonlinear excitation fields are controllably modulated between linear, circular, and various elliptical states. Polarization modulation is achieved by precise control over the time delay separating the orthogonal pulse pairs to within hundreds of attoseconds. The resultant emission from gold nanorods is imaged to a 2D array detector and correlated to the excitation field polarization and plasmon resonance frequency by Fourier transformation. Gold nanorods with length-to-diameter aspect ratios of 2 support a longitudinal surface plasmon resonance at approximately 800 nm, which is resonant with the excitation fundamental carrier wavelength. Differences in the intrinsic linear and circular dichroism resulting from variation in their relative alignment with respect to the laboratory frame enable optical differentiation of nanorods separated within 50 nm, which is an approximate 5-fold improvement over the diffraction limit of the microscope. The experimental results are supported by analytical simulations. In addition to subdiffraction spatial resolution, the vpFT-NLO method intrinsically provides the polarization- and frequency-dependent resonance response of the nanoparticles-providing spectroscopic information content along with super-resolution imaging capabilities.