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Time-correlated single photon Raman spectroscopy at megahertz repetition rates

MetadataDetails
Publication Date2021-07-08
JournalOptics Letters
AuthorsNeil Finlayson, Andrea Usai, Gillian E. Brown, Heather McEwan, Ahmet T. Erdogan
InstitutionsUniversity of Edinburgh
Citations8

Significant improvements in time-correlated single photon counting (TCSPC) Raman spectroscopy acquisition times can be achieved through exploitation of megahertz (MHz) laser repetition rates. We have developed a TCSPC Raman spectroscopy system based on a high peak power ( <mml:math xmlns:mml=ā€œhttp://www.w3.org/1998/Math/MathMLā€ display=ā€œinlineā€> <mml:mrow class=ā€œMJX-TeXAtom-ORDā€> <mml:mo>&gt;</mml:mo> </mml:mrow> <mml:mrow class=ā€œMJX-TeXAtom-ORDā€> <mml:mn>40</mml:mn> </mml:mrow> <mml:mspace width=ā€œthickmathspaceā€/> <mml:mrow class=ā€œMJX-TeXAtom-ORDā€> <mml:mi mathvariant=ā€œnormalā€>W</mml:mi> </mml:mrow> </mml:math> ) pulsed laser, a high pulse repetition rate (40 MHz), a custom <mml:math xmlns:mml=ā€œhttp://www.w3.org/1998/Math/MathMLā€ display=ā€œinlineā€> <mml:mrow class=ā€œMJX-TeXAtom-ORDā€> <mml:mi>f</mml:mi> </mml:mrow> <mml:mrow class=ā€œMJX-TeXAtom-ORDā€> <mml:mo>/</mml:mo> </mml:mrow> <mml:mrow class=ā€œMJX-TeXAtom-ORDā€> <mml:mn>1.5</mml:mn> </mml:mrow> </mml:math> spectrometer, and a 512 spectral channel Ɨ 16 time bin single photon avalanche diode line sensor. We report millisecond Raman spectrum acquisition times, a peak Raman count rate of 104 kcps, and a linewidth aggregated count rate of 440 kcps with a diamond sample. This represents a three-order-of-magnitude increase in measured Raman count rate in comparison with a 104 kHz pulsed laser operating at 300 W and a four-order-of-magnitude increase over a 0.1 W pulsed laser operating at 40 MHz. A Raman-to-fluorescence ratio of 4.76 is achieved with a sesame oil sample at a 20 MHz repetition rate. Achieving high count rates and Raman-to-fluorescence ratios unlocks the potential of combined Raman/fluorescence lifetime spectroscopy for imaging and other short acquisition time applications.

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