Comparability of Raman Spectroscopic Configurations: A Large Scale Cross-Laboratory Study

  • Anal Chem. 2020 Dec 15;92(24):15745-15756. doi: 10.1021/acs.analchem.0c02696.
Shuxia Guo  1  2 ,  Claudia Beleites  2  3 ,  Ute Neugebauer  1  2  4 ,  Sara Abalde-Cela  5 ,  Nils Kristian Afseth  6 ,  Fatima Alsamad  7 ,  Suresh Anand  8 ,  Cuauhtemoc Araujo-Andrade  9 ,  Sonja Aškrabić  10 ,  Ertug Avci  11 ,  Monica Baia  12 ,  Malgorzata Baranska  13  14 ,  Enrico Baria  15  16 ,  Luis A E Batista de Carvalho  17 ,  Philippe de Bettignies  18 ,  Alois Bonifacio  19 ,  Franck Bonnier  20 ,  Eva Maria Brauchle  21  22  23 ,  Hugh J Byrne  24 ,  Igor Chourpa  20 ,  Riccardo Cicchi  8  16 ,  Frederic Cuisinier  25 ,  Mustafa Culha  11 ,  Marcel Dahms  1  2  4 ,  Catalina David  18 ,  Ludovic Duponchel  26 ,  Shiyamala Duraipandian  24  27 ,  Samir F El-Mashtoly  28  29 ,  David I Ellis  30 ,  Gauthier Eppe  31 ,  Guillaume Falgayrac  32  33 ,  Ozren Gamulin  34  35 ,  Benjamin Gardner  36 ,  Peter Gardner  30  37 ,  Klaus Gerwert  28  29 ,  Evangelos J Giamarellos-Bourboulis  38 ,  Sveinbjorn Gizurarson  39 ,  Marcin Gnyba  40 ,  Royston Goodacre  41 ,  Patrick Grysan  42 ,  Orlando Guntinas-Lichius  43 ,  Helga Helgadottir  39 ,  Vlasta Mohaček Grošev  35  44 ,  Catherine Kendall  45 ,  Roman Kiselev  2  46 ,  Micha Kölbach  47 ,  Christoph Krafft  2 ,  Sivashankar Krishnamoorthy  42 ,  Patrick Kubryck  47 ,  Bernhard Lendl  48 ,  Pablo Loza-Alvarez  9 ,  Fiona M Lyng  24  27 ,  Susanne Machill  49 ,  Cedric Malherbe  31 ,  Monica Marro  9 ,  Maria Paula M Marques  17  50 ,  Ewelina Matuszyk  14 ,  Carlo Francesco Morasso  51 ,  Myriam Moreau  26 ,  Howbeer Muhamadali  41 ,  Valentina Mussi  52 ,  Ioan Notingher  53 ,  Marta Z Pacia  14 ,  Francesco S Pavone  15  16 ,  Guillaume Penel  32  33 ,  Dennis Petersen  29 ,  Olivier Piot  7  54 ,  Julietta V Rau  55  56 ,  Marc Richter  47 ,  Maria Krystyna Rybarczyk  57 ,  Hamideh Salehi  25 ,  Katja Schenke-Layland  21  22  23 ,  Sebastian Schlücker  58 ,  Markus Schosserer  59 ,  Karin Schütze  60 ,  Valter Sergo  19  61 ,  Faris Sinjab  53 ,  Janusz Smulko  40 ,  Ganesh D Sockalingum  7  54 ,  Clara Stiebing  2 ,  Nick Stone  36 ,  Valérie Untereiner  54 ,  Renzo Vanna  51 ,  Karin Wieland  48 ,  Jürgen Popp  1  2 ,  Thomas Bocklitz  1  2
Affiliations
  • 1. Institute of Physical Chemistry and Abbe Center of Photonics, University Jena, 07743 Jena, Germany.
  • 2. Member of Leibniz Health Technologies, Leibniz Institute of Photonic Technology Jena, 07745 Jena, Germany.
  • 3. Chemometrix GmbH, Södeler Weg 19, 61200 Wölfersheim, Germany.
  • 4. Center for Sepsis Control and Care, Jena University Hospital, Am Klinikum 1, D-07747 Jena, Germany.
  • 5. International Iberian Nanotechnology Laboratory (INL), Avda Mestre José Veiga, 4715-310 Braga, Portugal.
  • 6. Nofima - Norwegian Institute of Food, Fisheries and Aquaculture Research, NO-9291 Tromsø, Norway.
  • 7. Université de Reims Champagne-Ardenne, 51 rue Cognacq-Jay, BioSpecT-EA 7506, Reims, 51097 CEDEX, France.
  • 8. National Institute of Optics, National Research Council, 50019 Sesto Fiorentino, Italy.
  • 9. ICFO-Institut de Ciencies Fotoniques, The Barcelona Institute of Science and Technology, 08860 Castelldefels, Barcelona, Spain.
  • 10. Institute of Physics Belgrade, University of Belgrade, Studentski trg 1, Beograd, Serbia.
  • 11. Genetics and Bioengineering Department, Faculty of Engineering, Yeditepe University, Kayisdagi, 34755 Ataşehir/İstanbul, Turkey.
  • 12. Faculty of Physics, Babes-Bolyai University, Strada Mihail Kogǎlniceanu 1, Cluj-Napoca 400084, Romania.
  • 13. Faculty of Chemistry, Jagiellonian University, 2 Gronostajowa Str., 30-387 Krakow Poland.
  • 14. Jagiellonian Centre for Experimental Therapeutics (JCET), Michal̷a Bobrzyńskiego 14, 30-348 Kraków, Poland.
  • 15. Department of Physics, University of Florence, Piazza di San Marco, 4, 50121 Firenze FIorence, Italy.
  • 16. European Laboratory for Non-linear Spectroscopy, Via Nello Carrara, 1, 50019 Sesto Fiorentino FIorence, Italy.
  • 17. Molecular Physical Chemistry R&D Unit, Department of Chemistry, University of Coimbra, 3004-535 Coimbra, Portugal.
  • 18. HORIBA France SAS, 231 Rue de Lille, 59650 Villeneuve-d'Ascq, France.
  • 19. Raman Lab, Dept. Engineering and Architecture, University of Trieste, Via Alfonso Valerio, 6/1, 34127 Trieste, Italy.
  • 20. Faculty of pharmacy, EA6295 NanoMédicaments et Nanosondes, University of Tours, 60 Rue du Plat d'Étain, 37000 Tours, France.
  • 21. NMI Natural and Medical Sciences Institute at the University of Tübingen, Markwiesenstraße 55, 72770 Reutlingen, Germany.
  • 22. Department of Women's Health, Research Institute of Women's Health, Eberhard Karls University Tübingen, Geschwister-Scholl-Platz, 72074 Tübingen, Germany.
  • 23. Cluster of Excellence iFIT (EXC 2180) "Image-Guided and Functionally Instructed Tumor Therapies", Eberhard Karls University Tübingen, 72076 Tübingen, Germany.
  • 24. FOCAS Research Institute, Technological University Dublin, City Campus, Aungier St, Dublin, Ireland.
  • 25. LBN, University Montpellier, 641 Av. du Doyen Gaston Giraud, 34000 Montpellier, France.
  • 26. LASIRE - LAboratoire de Spectroscopie pour les Interactions, la Réactivité et l'Environnement, Univ. Lille, CNRS, UMR 8516 - F-59000 Lille, France.
  • 27. School of Physics & Clinical & Optometric Sciences, Technological University Dublin, City Campus, Kevin Street, Dublin 2, D08 X622, Ireland.
  • 28. Center for Protein Diagnostics (ProDi), Ruhr University Bochum, Gesundheitscampus 4, 44801 Bochum, Germany.
  • 29. Department of Biophysics, Faculty of Biology and Biotechnology, Ruhr University Bochum, Universitätsstraße 150, 44801 Bochum, Germany.
  • 30. Manchester Institute of Biotechnology, School of Chemistry, University of Manchester, M1 7DN, Manchester, United Kingdom.
  • 31. Mass Spectrometry Laboratory, MolSys Research Unit, University of Liege, Place du 20 Aoǔt 7, 4000 Liège, Belgium.
  • 32. MABLab, Marrow Adiposity and Bone Lab, Univ. Littoral Côte d'Opale, F-62300 Boulogne-sur-Mer, France.
  • 33. CHU Lille, 2 Avenue Oscar Lambret, F-59000 Lille, France.
  • 34. Department of Physics and Biophysics, School of Medicine, University of Zagreb, Šalata 3, 10000 Zagreb, Croatia.
  • 35. Centre for Advanced Materials Science, Bijenička 54, 10000 Zagreb, Croatia.
  • 36. Physics and Astronomy, Mathematics and Physical Sciences, College of Engineering, Exeter, EX4 4Q, United Kingdom.
  • 37. Department of Chemical Engineering and Analytical Science, School of Engineering, The University of Manchester, Manchester M1 3AL United Kingdom.
  • 38. 4th Department of Internal Medicine, National and Kapodistrian University of Athens, Medical School, 1 Rimini Str, Athens, Greece.
  • 39. Faculty of Pharmaceutical Sciences, University of Iceland, Reykjavik, Iceland.
  • 40. Faculty of Electronics, Telecommunications and Informatics, Gdańsk University of Technology, Gabriela Narutowicza 11/12, 80-233 Gdańsk, Poland.
  • 41. Department of Biochemistry and Systems Biology, Institute of Systems, Molecular and Integrative Biology, University of Liverpool, Liverpool L69 750 7ZB, United Kingdom.
  • 42. Materials Research and Technology, Luxembourg Institute of Science and Technology, 41, rue du Brill, L-4422 Belvaux, Luxembourg.
  • 43. Department of Otorhinolaryngology, Jena University Hospital, Bachstraße 18, 07743 Jena, Germany.
  • 44. Ruđer Bošković Institute, Bijenička 54, 10000 Zagreb, Croatia.
  • 45. Biophotonics Research Unit, Gloucestershire Hospitals NHS Foundation Trust, Leadon House, Great Western Rd, Gloucester GL1 3NN, United Kingdom.
  • 46. St. Jude Children's Research Hospital, 262 Danny Thomas Pl, Memphis, Tennessee 38105, United States.
  • 47. Renishaw GmbH, Karl-Benz-Straße 12, 72124 Pliezhausen Germany.
  • 48. Institute of Chemical Technologies and Analytics, TU Wien, 1040 Wien, Austria.
  • 49. Chair of Bioanalytical Chemistry, TU Dresden, 01062 Dresden, Germany.
  • 50. Department of Life Sciences, University of Coimbra, 3000-456 Coimbra, Portugal.
  • 51. Istituti Clinici Scientifici Maugeri IRCCS, Via Salvatore Maugeri, 10, 27100 Pavia, Italy.
  • 52. National Research Council, Institute for Microelectronics and Microsystems (IMM-CNR), Via del Fosso del Cavaliere, 100, 00133 Roma RM Rome, Italy.
  • 53. School of Physics and Astronomy, University of Nottingham, Nottingham NG7 2RD, United Kingdom.
  • 54. Université de Reims Champagne-Ardenne, PICT, 9 Boulevard de la Paix, 51097 Reims, France.
  • 55. Istituto di Struttura della Materia, Consiglio Nazionale delle Ricerche (ISM-CNR), Via del Fosso del Cavaliere, 100-00133 Rome, Italy.
  • 56. Sechenov First Moscow State Medical University, 119991 Moscow, Trubetskaya 8, build. 2, Russian Federation.
  • 57. Chemical Faculty, Gdansk University of Technology, 11/12 Narutowicza St., 80-233 Gdansk Poland.
  • 58. Faculty of Chemistry, University of Duisburg-Essen, Universitaetsstr. 5, 45141 Essen, Germany.
  • 59. Department of Biotechnology, Institute of Molecular Biotechnology, University of Natural Resources and Life Sciences, Gregor-Mendel-Straße 33, 1180 Vienna, Austria.
  • 60. CellTool GmbH, 82327 Tutzing, Germany.
  • 61. Faculty of Health Sciences, University of Macau, 999078 Macau, SAR China.
PMID: 33225709 DOI: 10.1021/acs.analchem.0c02696
Abstract

The variable configuration of Raman spectroscopic platforms is one of the major obstacles in establishing Raman spectroscopy as a valuable physicochemical method within real-world scenarios such as clinical diagnostics. For such real world applications like diagnostic classification, the models should ideally be usable to predict data from different setups. Whether it is done by training a rugged model with data from many setups or by a primary-replica strategy where models are developed on a 'primary' setup and the test data are generated on 'replicate' setups, this is only possible if the Raman spectra from different setups are consistent, reproducible, and comparable. However, Raman spectra can be highly sensitive to the measurement conditions, and they change from setup to setup even if the same samples are measured. Although increasingly recognized as an issue, the dependence of the Raman spectra on the instrumental configuration is far from being fully understood and great effort is needed to address the resulting spectral variations and to correct for them. To make the severity of the situation clear, we present a round robin experiment investigating the comparability of 35 Raman spectroscopic devices with different configurations in 15 institutes within seven European countries from the COST (European Cooperation in Science and Technology) action Raman4clinics. The experiment was developed in a fashion that allows various instrumental configurations ranging from highly confocal setups to fibre-optic based systems with different excitation wavelengths. We illustrate the spectral variations caused by the instrumental configurations from the perspectives of peak shifts, intensity variations, peak widths, and noise levels. We conclude this contribution with recommendations that may help to improve the inter-laboratory studies.

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