LIDAR SPRECTROSCOPY INSTRUMENT (LISSI): AN INFRASTRUCTURE FACILITY FOR CHEMICAL AEROSOL PROFILING AT THE UNIVERSITY OF HERTFORDSHIRE Matthias Tesche1,*, Boyan Tatarov1, Youngmin Noh2 and Detlef Müller1,2 1University of Hertfordshire, Hatfield, United Kingdom, ∗m.tesche@herts.ac.uk 2Gwangju Institute of Science and Technology, Gwangju, South Korea ABSTRACT The lidar development at the University of Hert- fordshire explores the feasibility of using Raman backscattering for chemical aerosol profiling. This paper provides an overview of the new facility. A high-power Nd:YAG/OPO setup is used to excite Raman backscattering at a wide range of wave- lengths. The receiver combines a spectrometer with a 32-channel detector or an ICCD camera to resolve Raman signals of various chemical compounds. The new facility will open new avenues for chemical profiling of aerosol pollution from measurements of Raman scattering by selected chemical compounds, provide data that allow to close the gap between op- tical and microphysical aerosol profiling with lidar and enables connecting lidar measurements to pa- rameters used in atmospheric modelling. 1 INTRODUCTION Conventional Raman or high spectral resolution li- dar is used for deriving profiles of aerosol optical properties and, if proper input data are provided, retrieving aerosol microphysical properties through inversion techniques. The lidar development at the University of Hertfordshire (UH) is centred on ex- ploring the feasibility of using Raman backscatter of various target species to obtain mass concentra- tion profiles of selected chemical compounds. This marks the logical next step in aerosol profiling with lidar and will allow for defining aerosol types ac- cording to their chemical composition rather than optical properties. Ultimately, this will unify the treatment of aerosol types in lidar remote sens- ing with that of in-situ measurements and atmo- spheric modelling. The feasibility of the underlying methodology has been proven for measurements of Raman backscattering at silicone dioxide molecules within Asian dust layers [1, 2, 3]. 2 OBJECTIVES The lidar spectroscopy instrument (LiSsI) will en- able profiling of trace gases, chemical components in particles, and bio-aerosols in atmospheric aerosol pollution through the combination of different non- linear spectroscopy techniques (photoluminescence, fluorescence, Raman and coherent anti-Stokes Ra- man spectroscopy) in a single measurement plat- form. The work at UH includes (1) the develop- ment of an end-to-end simulator that allows us to model the processes of inelastic photoluminescence and Raman scattering by aerosol particles and gases in the context of lidar remote sensing, (2) the iden- tification of the luminescence and Raman scatter- ing characteristics for a set of key aerosol types and gases (of natural and anthropogenic origin) by means of laboratory experiments, (3) test measure- ments and case studies as a proof of concept of the technique under laboratory conditions, and (4) the characterisation and development of a mobile pro- totype inelastic lidar spectrometer receiver for field deployment at established lidar sites. 3 LABORATORY SETUP Figure 1 presents a sketch of the setup of the LiSsI facility. The main components are a high power Nd:YAG laser (Continuum Powerlite Furie LD), an Optical Parametric Oscillator (Horizon OPO), a mo- torised beam combiner, a multiwavelength depolar- isation Raman lidar receiver, a Horiba 1250M spec- trometer that can be used with an intensified CCD camera (ICCD, Princeton Instruments PI-MAX4 1024i-HBf) or a 32-channel Licel PMT (32PMT), an Olympus BX51TRF-6 Raman/flourescence mi- croscope, and several custom-made gas chambers. An overview of the properties of the transmitter is provided in Table 1. The combination of a high- power Nd:YAG laser and an Optical Parametric Os- EPJ Web of Conferences 176, 01008 (2018) https://doi.org/10.1051/epjconf/201817601008 ILRC 28 © The Authors, published by EDP Sciences. This is an open access article distributed under the terms of the Creative Commons Attribution License 4.0 (http://creativecommons.org/licenses/by/4.0/). 192-400 nm 400-2750 nm 355, 532, 1064 nm P M T Nd:YAG laser OPO Telescope MBC Olympus BX51TRF-6 microscope gas chambers ICCD/32PMT Horiba 1250Mlidar receiver and data acquisition, signal selection for spectrometric measurements Figure 1: Sketch of the laboratory setup including a high-power Nd:YAG laser, a motorised beam combiner (MBC), an Optical Parametric Oscillator (OPO), an advanced lidar receiver, a spectrometer, an intensified CCD camera (ICCD), a 32-channel Licel PMT (32PMT), a Raman/flourescence microscope, and several gas chambers. cillator allows for exciting Raman backscatter for a wide range of excitation wavelengths. The novel li- dar receiver setup has been designed and simulated using ZEMAX and will combine the spectral res- olution of spectrometers with a 32-channel detec- tor to resolve Raman signals of a variety of chem- ical compounds. An overview of the configuration and properties of the receiver and data acquisition is provided in Table 2. Aerosol chambers will en- able measurements of a range of chemical species to test the methodology for known compounds and to assess the respective detection limit with respect to applied laser power and resolvable particle con- centrations. A Raman microscope will be used to measure the Raman scattering cross-sections of the selected target species—information that is needed to transform the detected signals into mass concen- trations. Table 1: Properties of the transmitter. Continuum Powerlite Furie LD Laser type Nd:YAG, injection seeded Wavelength and 7500mJ @1064 nm pulse energy 5000mJ @532 nmnm 2500mJ @355 nm Beam divergence 0.5mrad, 0.1mrad after 5-fold beam expansion Repetition rate 10Hz Linewidth <0.003 cm−1 Pulse duration <15 ns Horizon Optical Parametric Oscillator Pumping wavelength 355 nm Wavelength and from 192 to 2750 nm pulse energy scanning step 0.01 nm 120mJ @400 nm 60mJ @600 nm 25mJ @300 nm Beam divergence <2mrad (both axes) Repetition rate 10Hz Linewidth 2-6 cm−1, injection seeded Pulse duration <15 ns The aim of the facility is to carry out precise inelas- tic spectroscopy experiments that target measure- ments of photoluminescence, fluorescence, and Ra- man spectra of aerosol and gas samples. These mea- surements will include the identification of spec- tra, absolute values of fluorescence, and Raman cross-sections that are currently poorly known or unknown. 4 APPLICATIONS IN LIDAR AND SPEC- TROSCOPY The LiSsI facility has been designed to allow for comprehensive laboratory experiments as well as for atmospheric observations. The laser beam can be released into the atmosphere through a hatch in the roof of the laboratory. The backscattered light is collected with a 14-inch Schmidt-Cassegrain tele- scope and guided to the different components of the receiver (Table 2). Depending on the setup of the experiment, LiSsI can be used as multi- wavelength elastic backscatter lidar for measure- ments of aerosols and temperature from the tropo- sphere to the mesosphere, as multi-channel spectro- scopic Raman lidar (using Stokes and anti-Stokes, rotational, and rotational-vibrational Raman scat- tering), multi-channel spectroscopic photolumines- cence/fluorescence lidar, high spectral resolution li- 2 EPJ Web of Conferences 176, 01008 (2018) https://doi.org/10.1051/epjconf/201817601008 ILRC 28 192-400 nm 400-2750 nm 355, 532, 1064 nm P M T Nd:YAG laser OPO Telescope MBC Olympus BX51TRF-6 microscope gas chambers ICCD/32PMT Horiba 1250Mlidar receiver and data acquisition, signal selection for spectrometric measurements Figure 1: Sketch of the laboratory setup including a high-power Nd:YAG laser, a motorised beam combiner (MBC), an Optical Parametric Oscillator (OPO), an advanced lidar receiver, a spectrometer, an intensified CCD camera (ICCD), a 32-channel Licel PMT (32PMT), a Raman/flourescence microscope, and several gas chambers. cillator allows for exciting Raman backscatter for a wide range of excitation wavelengths. The novel li- dar receiver setup has been designed and simulated using ZEMAX and will combine the spectral res- olution of spectrometers with a 32-channel detec- tor to resolve Raman signals of a variety of chem- ical compounds. An overview of the configuration and properties of the receiver and data acquisition is provided in Table 2. Aerosol chambers will en- able measurements of a range of chemical species to test the methodology for known compounds and to assess the respective detection limit with respect to applied laser power and resolvable particle con- centrations. A Raman microscope will be used to measure the Raman scattering cross-sections of the selected target species—information that is needed to transform the detected signals into mass concen- trations. Table 1: Properties of the transmitter. Continuum Powerlite Furie LD Laser type Nd:YAG, injection seeded Wavelength and 7500mJ @1064 nm pulse energy 5000mJ @532 nmnm 2500mJ @355 nm Beam divergence 0.5mrad, 0.1mrad after 5-fold beam expansion Repetition rate 10Hz Linewidth <0.003 cm−1 Pulse duration <15 ns Horizon Optical Parametric Oscillator Pumping wavelength 355 nm Wavelength and from 192 to 2750 nm pulse energy scanning step 0.01 nm 120mJ @400 nm 60mJ @600 nm 25mJ @300 nm Beam divergence <2mrad (both axes) Repetition rate 10Hz Linewidth 2-6 cm−1, injection seeded Pulse duration <15 ns The aim of the facility is to carry out precise inelas- tic spectroscopy experiments that target measure- ments of photoluminescence, fluorescence, and Ra- man spectra of aerosol and gas samples. These mea- surements will include the identification of spec- tra, absolute values of fluorescence, and Raman cross-sections that are currently poorly known or unknown. 4 APPLICATIONS IN LIDAR AND SPEC- TROSCOPY The LiSsI facility has been designed to allow for comprehensive laboratory experiments as well as for atmospheric observations. The laser beam can be released into the atmosphere through a hatch in the roof of the laboratory. The backscattered light is collected with a 14-inch Schmidt-Cassegrain tele- scope and guided to the different components of the receiver (Table 2). Depending on the setup of the experiment, LiSsI can be used as multi- wavelength elastic backscatter lidar for measure- ments of aerosols and temperature from the tropo- sphere to the mesosphere, as multi-channel spectro- scopic Raman lidar (using Stokes and anti-Stokes, rotational, and rotational-vibrational Raman scat- tering), multi-channel spectroscopic photolumines- cence/fluorescence lidar, high spectral resolution li- 2 Table 2: Properties of the receiver and data acquisition system. Schmidt-Cassegrain telescope Focal length 3910mm (14 inch) Field of view 0.5-4.0mrad (variable) HORIBA 1250M Research Spectrometer Focal length 1.25m Aperture F/9 Spectral range 0-1500 nm mechanical range (1200 g/mm grating) Grating size 110mm × 110mm Dispersion @500 nm 0.65 nm/mm Accuracy ±0.15 nm Repeatability ±0.005 nm Gratings 2400 g/mm blaze 250 nm, max resolution 0.003 nm and resolutions 1800 g/mm blaze 400 nm, max resolution 0.004 nm @313.183 nm 1200 g/mm blaze 330 nm, max resolution 0.006 nm 600 g/mm blaze 500 nm, max resolution 0.012 nm Detection Mie and Rayleigh 355 nm, PMT HV-R9880U-20, bandwidth 1.3 nm scattering 532 nm, PMT HV-R9880U-20, bandwidth 1.3 nm 1064 nm, APD InGaAs50, bandwidth 4 nm Spectroscopic 1 Hamamatsu H7260-20, 0.8mm×7mm×32 anodes Licel SP32-20 spectral response 300-920 nm Spectroscopic 2 1024×1024 imaging pixels; 12.8 µm×12.8 µm pixels Princeton Instruments Gen III filmless intensifier PI-MAX4 Sensitive range 290-710 nm ICCD camera QE>20% in range 355-700 nm; QE>40% in range 410-640 nm Data acquisition system Mie and Rayleigh Licel transient recorders, 16 bit, 20MHz A/D converters and photon-counters scattering maximum count rate 250MHz, variable range resolution Multi-anode PMT Single-photon counting system, maximum count rate 100MHz, 50 ns resolution ICCD Digitization 16 bit, 32MHz, minimum gate width 2 ns dar (HSRL), polarization lidar, or infrared absorp- tion and differential absorption lidar (DIAL). In addition, LiSsI opens possibilities for a wide range of applications in spectroscopy: general spectroscopy (attenuation, transmission, and re- flectance spectroscopy), high-spectral resolution spectroscopy, Stokes and anti-Stokes Raman spec- troscopy of gas and solid material including ap- plications involving a microscope, fluorescence spectroscopy of gas and solid material including microscope applications, laser-induced breakdown spectroscopy, coherent-anti-Stokes Raman spec- troscopy, time-resolved spectroscopy, infrared gas analysis and materials processing. 5 FIRST RESULTS The LiSsI laser has been installed in September 2017. Figure 2 shows one of the first measure- 1E6 Figure 2: First measurement at 532 nm on 22 September 2017 (black) together with a molecular (red) and a temperature (blue) profile from a sounding launched at Nottingham at 0000 UTC on 22 September 2017. ments performed between 1026 and 1330 UTC on 22 September 2017 using only a 532-nm elastic channel and a laser power of about 30mJ. The ana- log counting signal is shown in the figure. Despite the low laser power, a rather small telescope and 3 EPJ Web of Conferences 176, 01008 (2018) https://doi.org/10.1051/epjconf/201817601008 ILRC 28                            Figure 3: Time-height display (left) and average profile (right) of the range-corrected signed at 532 nm detected during a measurement between 1644 and 2010 UTC on 28 September 2017 with a temporal resolution of one minute. observations being performed during daytime, rea- sonable signals can be obtained up to a height of 20 km. Aerosol can be seen in the lowermost 4 km as well as in layers at 7, 11, 14, 15, and 16 km height. The temperature profile of a radiosonde launched at Nottingham (about 150 km north of Hat- field) shows the tropospause at about 10 km height, putting the upper aerosol layers—likely originating from pyro-cumulonimbus events in Canada several weeks earlier—well within the stratosphere. Figure 3 presents data from the first nighttime mea- surement performed with LiSsI. The configuration has been the same as during the measurements pre- sented in Figure 2. Cirrus clouds are clearly visible between 6.5 and 13.0 km. The stratospheric aerosol layer from Figure 2 is still present between 17 and 18 km height. 6 NEXT MILESTONES The coming milestones in developing the LiSsI fa- cility are aligned with increasing the complexity of the optical setup. After the initial test measurements (Figure 2), we intend to perform atmospheric mea- surements of elastically and inelastically backscat- tered light at the different laser wavelength using full power. After that, the spectrometer will be inte- grated into the lidar receiver to allow for multispec- tral measurements in the atmosphere and using the gas and aerosol chambers in the laboratory. ACKNOWLEDGEMENTS The LiSsI facility has been funded by the Uni- versity of Hertfordshire through capital investment. Boyan Tatarov is supported by a Marie Skłodowska- Curie Action Fellowship of the European Commis- sion (CAPABLE, H2020-MSCA-IF-2015). References [1] Tatarov, B. and Sugimoto, N., 2005: Estimation of quartz concentration in the tropospheric mineral aerosols using combined Raman and high spectral resolution lidars, Opt. Lett. 30, 3407-3409. [2] Müller et al., 2010: Mineral quartz concentration measurements of mixed mineral dust/urban haze pollution plumes over Korea with multiwavelength aerosol Raman-quartz lidar,Geophys. Res. Lett. 37, 2010GL044633. [3] Tatarov et al., 2011: Lidar measurements of Ra- man scattering at ultraviolet wavelength from min- eral dust over East Asia, Opt. Expr. 19, 1569-1581. 4 EPJ Web of Conferences 176, 01008 (2018) https://doi.org/10.1051/epjconf/201817601008 ILRC 28