Nanospectroscopy, using the apertureless scattering method, has become a standard method for achieving spectral analysis of surfaces with spatial resolution approaching 10 nm. The method involves light scattered from the tip of an atomic force microscope (AFM) in combination with a Michelson-type interferometer and infrared detector. A high spectral radiance source (such as a laser) is necessary for overcoming the extremely small scattering efficiency. Examples include the quantum cascade laser (QCL), although having somewhat limited spectral coverage. Here we describe our capabilities at the National Synchrotron Light Source II (NSLS II) using a truly broadband (continuum) source of synchrotron infrared to perform FTIR spectroscopy into the far-IR. A key component for achieving this is a long-wavelength MCT photoconductor operating at T=4.2K and reaching wavelengths beyond 50 microns (i.e. below 200 cm-1). Results showing polaritons in 2D materials as well as semiconductor transport characterization will be included.
*This work supported by the U.S. DOE under contract DE-SC0012704 at NSLS-II and BNL.
The Neaspec SNOM used in this work provided courtesy of Attocube GmbH.
We describe the performance of long-wavelength MCT operating at 4.2K as a fast photoconductive detector for far-infrared nanospectroscopy. The technique employs scattering from the tip of an atomic force microscope (AFM) engaged with a sample surface while in "tapping mode" at a frequency f, with the scattered infrared sensed at a higher harmonic, e.g. 2f, 3f or even 4f to improve spatial discrimination. With typical tapping frequencies >100 kHz, the infrared detector requires a bandwidth of 1 MHz or higher, for which thermal-type IR detectors are not sufficiently fast. MCT detectors are usually limited to wavelengths shorter than 25µm when operating at T=77K, but this can be overcome by cooling to 4.2K, in which case the detection threshold wavelength extends to beyond 50 microns. An additional benefit is an overall 5X improvement in S/N.
*This work supported by the U.S. Department of Energy under contract DE-SC0012704 at NSLS-II and BNL.
See ACS Photonics, 10, 4329-4339 (2023), (https://doi.org/10.1021/acsphotonics.3c01148)
High contrast imaging can use pupil apodizers to suppress diffracted starlight from a bright source in order to observe its environs. Metallic half-tone dot transmissive apodizers were developed for the Gemini Planet Imager (GPI) and ESO SPHERE coronagraphs for use in the near-IR. Dot sizes on the scale of the wavelength of the light often result in unexpected variations in the optical transmission vs. superficial dot density relation. We measured 5 and 10 micron half-tone microdot screens' transmissions between 550 -1050 nm to prepare to fabricate apodizations that mitigate diffraction by segments gaps and spiders on future large space telescopes. We utilized slow test beams (f/40, f/80) to estimate the on-axis (far-field, or zero-order) transmission of test patches using a Fourier Transform Spectrograph on Beamline U10B at Brookhaven National Laboratory's National Synchrotron Light Source (BNL NSLS). We also modified our previous GPI IR characterization hardware and methods for this experiment. Our measurements show an internal consistency of 0.1% in transmission, a factor of 5 better than our near-IR GPI work on the NSLS U4IR beamline. The systematics of the set-up appeared to limit the absolute calibration for our f/40 data on the 50-patch, maximum Optical Density 3 (OD3), sample. Credible measurements of transmissions down to about 3% transmission were achieved for this sample. Future work on apodizers for obstructed and segmented primary mirror coronagraphs will require configurations that mimic the intended diffractive configurations closely in order to tune apodizer fabrication to any particular application, and measure chromatic effects in representative diffractive regimes. Further experimental refinements are needed to measure the densest test patches which possess transmissions less than a few percent. The new NSLS-II should provide much greater spectral stability of its synchrotron beam, which will improve measurement accuracy and reduce systematics.
The Gemini Planet Imager (GPI) is an extreme AO coronagraphic integral field unit YJHK spectrograph destined
for first light on the 8m Gemini South telescope in 2011. GPI fields a 1500 channel AO system feeding an
apodized pupil Lyot coronagraph, and a nIR non-common-path slow wavefront sensor. It targets detection and
characterizion of relatively young (<2GYr), self luminous planets up to 10 million times as faint as their primary
star. We present the coronagraph subsystem's in-lab performance, and describe the studies required to specify
and fabricate the coronagraph. Coronagraphic pupil apodization is implemented with metallic half-tone screens
on glass, and the focal plane occulters are deep reactive ion etched holes in optically polished silicon mirrors. Our
JH testbed achieves H-band contrast below a million at separations above 5 resolution elements, without using
an AO system. We present an overview of the coronagraphic masks and our testbed coronagraphic data. We
also demonstrate the performance of an astrometric and photometric grid that enables coronagraphic astrometry
relative to the primary star in every exposure, a proven technique that has yielded on-sky precision of the order
of a milliarsecond.
High contrast imaging sometimes uses apodized masks in coronagraphs to suppress diffracted starlight from
a bright source in order to observe its environs. Continuously graded opacity material and metallic half-tone
dots are two possible apodizers fabrication techniques. In the latter approach if dot sizes are comparable to the
wavelength of the light, surface plasmon effects can complicate the optical density (OD) vs. superficial dot density
relation. OD can also be a complicated function of wavelength. We measured half-tone microdot screens' and
continuous materials' transmissions. Our set-up replicated the f/ 64 optical configuration of the Gemini Planet
Imager's Apodized Pupil Lyot Coronagraph pupil plane, where we plan to place our pupil plane masks. Our
half-tone samples were fabricated with 2, 5, and 10 micron dot sizes, our continuous greyscale was High Energy
Electron Beam Sensitive (HEBS) glass (Canyon Materials Inc.). We present optical density (OD) vs. wavelength
curves for our half-tone and continuous greyscale samples 1.1 - 2.5 μm wavelength range. Direct measurements
of the beam intensity in the far field using a Fourier Transform Infrared Spectrograph on Beamline U4IR at
Brookhaven National Laboratory's National Synchrotron Light Source (NSLS) provided transmission spectra of
test patches and apodizers. We report the on-axis IR transmission spectra through screens composed of metallic
dots that are comparable in size with the wavelength of the light used, over a range of optical densities. We also
measured departures from simple theory describing the array of satellite spots created by thin periodic grids in
the pupil of the system. Such spots are used for photometry and astrometry in coronagraphic situations. Our
results pertain to both ground and space based coronagraphs that use spatially variable attenuation, typically
in focal plane or pupil plane masks.
Coherent synchrotron radiation from the NSLS VUV ring has been detected and partially characterized. The observations have been performed at the new far infrared beamline U12IR. The coherent radiation is peaked near a wavelength of 7 mm and occurs in short duration bursts. The bursts occur only when the electron beam current (I) exceeds a threshold value (Ith), which itself varies with ring operating conditions. Beyond threshold, the average intensity of the emission is found to increase as (I-Ith)2. The coherent emission implies micro-bunching of the electron beam due to a longitudinal instability.
A facility for performing time-resolved infrared spectroscopy has been developed at the NSLS, primarily at beamline U12IR. The pulsed IR light from the synchrotron is used to perform pump-probe spectroscopy. We present here a description of the facility and results for the relaxation of photoexcitations in both a semiconductor and superconductor.
The UV-storage ring Free Electron Laser (FEL) operating at Super-ACO is a tunable, coherent and intense (up to 300 mW) photon source in the near-UV range (300 - 350 nm). Besides, it has the unique feature to be synchronized in a one-to-one shot ratio with the Synchrotron Radiation (SR) at the high repetition rate of 8.32 MHz. This FEL + SR combination appears to be very powerful for the performance of pump- probe time-resolved and/or frequency-resolved experiments on the sub-ns and ns time-scales. In particular, there is a strong scientific case for the combination of the recently- commissioned SA5 Infra-Red Synchrotron Radiation beamline with the UV-FEL, for the performance of transient IR- absorption spectroscopy on FEL-excited samples with a Fourier-transform spectrometer coupled with a microscope allowing high spectral and spatial resolution. The principle and interest of the two-color combination altogether with the description of both the FEL and the SA5 IR beamline are presented. The first synchronization signal between the IR and the UV beams is shown. The correct spatial overlap between the UV (FEL) and the IR (SR) photon beams is demonstrated by monitoring via IR-spectro-microscopy the time evolution of a single mineral particulate (kaolinite) under UV-FEL irradiation.
The first of several new infrared beamlines, built on a modified bending magnet port of the NSLS VUV ring, is now operational for mid-infrared microspectroscopy. The port simultaneously delivers 40 mrad by 40 mrad to two separate beamlines and spectrometer endstations designated U10A and U10B. The latter is equipped with a scanning infrared microspectrometer. The combination of this instrument and high brightness synchrotron radiation makes diffraction- limited microspectroscopy practical. This paper describes the beamline's performance and presents quantitative information on the diffraction-limited resolution.
Infrared Microspectroscopy, using a globar source, is now widely employed in the industrial environment, for the analysis of various materials. Since synchrotron radiation is a much brighter source, an enhancement of an order of magnitude in lateral resolution can be achieved. Thus, the combination of IR microspectroscopy, and synchrotron radiation provides a powerful tool enabling sample regions only few microns size to be studied. This opens up the potential for analyzing small particles. Some examples for hair, bitumen and polymer are presented.
Infrared microspectroscopy with a high brightness synchrotron source can achieve a spatial resolution approaching the diffraction limit. However, in order to realize this intrinsic source brightness at the specimen location, some care must be taken in designing the optical system. Also, when operating in diffraction limited conditions, the effective spatial resolution is no longer controlled by the apertures typically used for a conventional (geometrically defined) measurement. Instead, the spatial resolution depends on the wavelength of light and the effective apertures of the microscope's Schwarzchild objectives. We have modeled the optical system from the synchrotron source up to the sample location and determined the diffraction-limited spatial distribution of light. Effects due to the dependence of the synchrotron source's numerical aperture on wavelength, as well as the difference between transmission and reflection measurement modes, are also addressed. Lastly, we examine the benefits (when using a high brightness source) of an extrinsic germanium photoconductive detector with cone optics as a replacement for the standard MCT detector.
Infrared microspectroscopy combines microscopy and spectroscopy for the purpose of chemical microanalysis. Light microscopy provides a way to generate and record magnified images and visibly resolve microstructural detail. Infrared spectroscopy provides a means for analyzing the chemical makeup of materials. Combining light microscopy and infrared spectroscopy permits the correlation of microstructure with chemical composition. Inherently, the long wavelengths of infrared radiation limit the spatial resolution of the technique. However, synchrotron infrared radiation significantly improves both the spectral and spatial resolution of an infrared microspectrometer, such that data can be obtained with high signal-to-noise at the diffraction limit, which is 3 - 5 micrometers in the mid-infrared region.
Chemical mapping of proteins and lipids inside a single living cell and at a resolution of a few microns, has been performed using synchrotron infrared microspectrometry. Modifications of the chemical distributions upon mitosis and necrosis has been investigated.
Electron synchrotron storage rings, such as the VUV ring at the National Synchrotron Light Source, product short pulses of IR radiation suitable for investigating time-dependent phenomena in a variety of interesting experimental systems. In contrast to other pulsed sources of IR, the synchrotron produces a continuum spectral output over the entire IR (and beyond), though at power levels typically below those obtained from laser systems. The infrared synchrotron radiation source is therefore well-suited as a probe using standard FTIR spectroscopic techniques. Here we describe the pump-probe spectroscopy facility being established at the NSLS and demonstrate the technique by measuring the photocarrier decay in a semiconductor.
The transient thermal photoresponse of YBCO thin epitaxial films is calculated for conditions comparable to those frequently used in actual photoresponse measurements. At low light fluences and low bias currents, the calculations are in accord with a linear bolometric response. At higher fluences and bias currents, the thermal response displays behaviors often attributed to a non-bolometric mechanism. This is particularly true for the response decay time, which can decrease as the temperature falls through Tc. Some comparisons with experiment are presented, and it is concluded that a careful analysis is required to distinguish non-bolometric from bolometric response, especially for conditions of high light fluence.
Electron synchrotrons can serve as infrared sources with special characteristics which are particularly well matched to certain types of experiments. The electrons emit from a small area into a narrow solid angle, resulting in a source several orders of magnitude brighter (and at very long wavelengths, greater overall power) than a blackbody source. The NSLS infrared beamline at Brookhaven National Laboratory realizes these advantages, and the source has been used to explore, among other things, the properties of high-Tc copper oxide superconductors.
We report studies of a thin high-Ta film operating as a fast bolometric detector of infrared radiation. The film has a response of several mV when exposed to a 1 W, 1 ns duration broadband infrared pulse. The decay after the pulse was about 4 ns. The temperature dependence of the response accurately tracked dR/dT. A thermal model, in which the film's temperature varies relative to the substrate, provides a good description of the response. We find no evidence for other (non-bolometric) response mechanisms for temperatures near or well below T.
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