Transient absorption (TA) spectroscopy is considered as a powerful technique that reflects the ultrafast dynamics of photogenerated carriers in photoelectric and photocatalysis materials. However, limited by its sensitivity, the photogenerated carrier density in TA measurements of solar energy materials is usually much higher than that in the real working condition. Here, we present a combination of kHz macro-pulse and MHz micro-pulse technique for an ultrahigh sensitive TA spectrometer, which improves the sensitivity to the 10−7 level of ΔOD. It enables us to study ultrafast carrier dynamics pumped by very low power, which can avoid the influence of many-body interactions and the nonlinear effect associated with high carrier density. This work provides a novel TA method with ultrahigh sensitivity, which will play an important role in investigating the carrier dynamics of semiconductors in the working condition.

1.
K. E.
Knowles
,
M. D.
Koch
, and
J. L.
Shelton
,
J. Mater. Chem. C
6
,
11853
11867
(
2018
).
2.
R.
Berera
,
R.
van Grondelle
, and
J. T. M.
Kennis
,
Photosynth. Res.
101
,
105
118
(
2009
).
3.
K.
Wu
,
G.
Liang
,
Q.
Shang
,
Y.
Ren
,
D.
Kong
, and
T.
Lian
,
J. Am. Chem. Soc.
137
,
12792
12795
(
2015
).
4.
K.
Ishioka
,
B. G.
Barker
,
M.
Yanagida
,
Y.
Shirai
, and
K.
Miyano
,
J. Phys. Chem. Lett.
8
,
3902
(
2017
).
5.
S.
Kahmann
and
M. A.
Loi
,
J. Mater. Chem. C
7
,
2471
2486
(
2019
).
6.
7.
L. M.
Herz
,
ACS Energy Lett.
2
,
1539
1548
(
2017
).
8.
V. I.
Klimov
and
D. W.
McBranch
,
Opt. Lett.
23
,
277
279
(
1998
).
9.
S. V.
Frolov
and
Z. V.
Vardeny
,
Rev. Sci. Instrum.
69
,
1257
1260
(
1998
).
10.
C.
Schriever
,
S.
Lochbrunner
,
E.
Riedle
, and
D. J.
Nesbitt
,
Rev. Sci. Instrum.
79
,
013107
(
2008
).
11.
A. L.
Dobryakov
,
S. A.
Kovalenko
,
A.
Weigel
,
J. L.
Pérez-Lustres
,
J.
Lange
,
A.
Müller
, and
N. P.
Ernsting
,
Rev. Sci. Instrum.
81
,
113106
(
2010
).
12.
G.
Auböck
,
C.
Consani
,
R.
Monni
,
A.
Cannizzo
,
F.
van Mourik
, and
M.
Chergui
,
Rev. Sci. Instrum.
83
,
093105
(
2012
).
13.
B.
Lang
,
Rev. Sci. Instrum.
89
,
093112
(
2018
).
14.
S. D.
Stranks
,
V. M.
Burlakov
,
T.
Leijtens
,
J. M.
Ball
,
A.
Goriely
, and
H. J.
Snaith
,
Phys. Rev. Appl.
2
,
034007
(
2014
).
15.
S. M.
Sze
and
K. K.
Ng
,
Physics of Semiconductor Devices
(
John Wiley & Sons
,
NJ
,
2006
).
16.
V.
D’Innocenzo
,
G.
Grancini
,
M. J. P.
Alcocer
,
A. R. S.
Kandada
,
S. D.
Stranks
,
M. M.
Lee
,
G.
Lanzani
,
H. J.
Snaith
, and
A.
Petrozza
,
Nat. Commun.
5
,
3586
(
2014
).
17.
J.
Shi
,
Y.
Li
,
Y.
Li
,
D.
Li
,
Y.
Luo
,
H.
Wu
, and
Q.
Meng
,
Joule
2
,
879
901
(
2018
).
18.
R.
Wang
,
L.
Chen
,
Y.
Zhao
, and
G.
Jin
,
Rev. Sci. Instrum.
91
,
073101
(
2020
).
19.
N. T.
Hunt
,
A. A.
Jaye
, and
S. R.
Meech
,
Phys. Chem. Chem. Phys.
9
,
2167
2180
(
2007
).
20.
E. C.
Robinson
,
J.
Trägårdh
,
I. D.
Lindsay
, and
H.
Gersen
,
Rev. Sci. Instrum.
83
,
063705
(
2012
).
21.
R. J.
Deri
and
R.
Welter
,
Electron. Lett.
29
,
75
(
1993
).
22.
M. A.
Green
,
Y.
Hishikawa
,
E. D.
Dunlop
,
D. H.
Levi
,
J.
Hohl-Ebinger
, and
A. W. Y.
Ho-Baillie
,
Prog. Photovolt. Res. Appl.
26
,
427
436
(
2018
).
23.
D.
Kuciauskas
,
J.
Moseley
,
P.
Ščajev
, and
D.
Albin
,
Phys. Status Solidi RRL
14
,
1900606
(
2020
).
24.
M.
Okano
,
L. Q.
Phuong
, and
Y.
Kanemitsu
,
Phys. Status Solidi B
252
,
1219
1224
(
2015
).
25.
P.
Ščajev
,
S.
Miasojedovas
,
A.
Mekys
,
D.
Kuciauskas
,
K. G.
Lynn
,
S. K.
Swain
, and
K.
Jarašiūnas
,
J. Appl. Phys.
123
,
025704
(
2018
).
26.
B.
Pandit
,
R.
Dharmadasa
,
I. M.
Dharmadasa
,
T.
Druffel
, and
J.
Liu
,
Phys. Chem. Chem. Phys.
17
,
16760
16766
(
2015
).
27.
N.
Shrestha
,
C. R.
Grice
,
E.
Bastola
,
G. K.
Liyanage
,
A. B.
Phillips
,
M. J.
Heben
,
Y.
Yan
, and
R. J.
Ellingson
,
MRS Adv.
3
,
3293
3299
(
2018
).
28.
D.
Kuciauskas
,
P.
Dippo
,
Z.
Zhao
,
L.
Cheng
,
A.
Kanevce
,
W. K.
Metzger
, and
M.
Gloeckler
,
IEEE J. Photovolt.
6
,
313
318
(
2016
).
29.
J. M.
Kephart
,
A.
Kindvall
,
D.
Williams
,
D.
Kuciauskas
,
P.
Dippo
,
A.
Munshi
, and
W. S.
Sampath
,
IEEE J. Photovolt.
8
,
587
593
(
2018
).
30.
P.
Horodyský
and
P.
Hlídek
,
Phys. Status Solidi B
243
,
494
501
(
2006
).
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