Dual-Frequency Comb Transient Absorption: Broad Dynamic Range Measurement of Femtosecond to Nanosecond Relaxation Processes

Jun Woo Kim, Byungmoon Cho, Tai Hyun Yoon, Minhaeng Cho

Research output: Contribution to journalArticle

11 Citations (Scopus)

Abstract

We experimentally demonstrate a dual-frequency comb-based transient absorption (DFC-TA) technique, which has a 12 fs time resolution and an ultrafast scan rate. Here, the fast scan rate is achieved by employing asynchronous optical sampling (ASOPS), which utilizes two independent mode-locked lasers with a slightly detuned repetition rates. The ASOPS approach is advantageous because photodegradation damage of optical sample during TA measurements can be minimized by a gated sampling. We show that the vibrational and electronic population relaxations of near-IR dye molecules in solution that occur in the time range from femtoseconds to nanoseconds can be resolved even with a single time scan measurement. The phase coherent nature of our dual-frequency comb lasers is shown to be the key for successful coherent averaging with femtosecond time resolution preserved over many data acquisitions. We anticipate that the present DFC-TA method without using any pump-probe time delay devices could be of use in developing ultrafast TA-based microscopy and time-resolved coherent multidimensional spectroscopy.

Original languageEnglish
Pages (from-to)1866-1871
Number of pages6
JournalJournal of Physical Chemistry Letters
Volume9
Issue number8
DOIs
Publication statusPublished - 2018 Apr 19

ASJC Scopus subject areas

  • Materials Science(all)

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