TY - JOUR
T1 - Dual-Frequency Comb Transient Absorption
T2 - Broad Dynamic Range Measurement of Femtosecond to Nanosecond Relaxation Processes
AU - Kim, Jun Woo
AU - Cho, Byungmoon
AU - Yoon, Tai Hyun
AU - Cho, Minhaeng
PY - 2018/4/19
Y1 - 2018/4/19
N2 - 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.
AB - 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.
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U2 - 10.1021/acs.jpclett.8b00886
DO - 10.1021/acs.jpclett.8b00886
M3 - Article
C2 - 29589950
AN - SCOPUS:85045732474
VL - 9
SP - 1866
EP - 1871
JO - Journal of Physical Chemistry Letters
JF - Journal of Physical Chemistry Letters
SN - 1948-7185
IS - 8
ER -