Title: Breaking Barriers in Ultrafast Spectroscopy and Imaging Using 100 kHz Amplified Yb-Laser Systems

Abstract

Ultrafast spectroscopy and imaging have become tools utilized by a broad range of scientists involved in materials, energy, biological, and chemical sciences. Commercialization of ultrafast spectrometers including transient absorption spectrometers, vibrational sum frequency generation spectrometers, and even multidimensional spectrometers have put these advanced spectroscopy measurements into the hands of practitioners originally outside the field of ultrafast spectroscopy. There is now a technology shift occurring in ultrafast spectroscopy, made possible by new Yb-based lasers, that is opening exciting new experiments in the chemical and physical sciences. Amplified Yb-based lasers are not only more compact and efficient than their predecessors but also, most importantly, operate at many times the repetition rate with improved noise characteristics in comparison to the previous generation of Ti:sapphire amplifier technologies. Taken together, these attributes are enabling new experiments, generating improvements to long-standing techniques, and affording the transformation of spectroscopies to microscopies. This Account aims to show that the shift to 100 kHz lasers is a transformative step in nonlinear spectroscopy and imaging, much like the dramatic expansion that occurred with the commercialization of Ti:sapphire laser systems in the 1990s. The impact of this technology will be felt across a great swath of scientific communities. We first describemore » the technology landscape of amplified Yb-based laser systems used in conjunction with 100 kHz spectrometers operating with shot-to-shot pulse shaping and detection. We also identify the range of different parametric conversion and supercontinuum techniques which now provide a path to making pulses of light optimal for ultrafast spectroscopy. Second, we describe specific instances from our laboratories of how the amplified Yb-based light sources and spectrometers are transformative. For multiple probe time-resolved infrared and transient 2D IR spectroscopy, the gain in temporal span and signal-to-noise enables dynamical spectroscopy measurements from femtoseconds to seconds. These gains widen the applicability of time-resolved infrared techniques across a range of topics in photochemistry, photocatalysis, and photobiology as well as lower the technical barriers to implementation in a laboratory. For 2D visible spectroscopy and microscopy with white light, as well as 2D IR imaging, the high repetition rates of these new Yb-based light sources allow one to spatially map 2D spectra while maintaining high signal-to-noise in the data. To illustrate the gains, we provide examples of imaging applications in the study of photovoltaic materials and spectroelectrochemistry.« less

Authors:

Donaldson, Paul M.  ^[1];

• Search DOE PAGES for author "Donaldson, Paul M."
• Search DOE PAGES for ORCID "0000-0002-0305-9142"

Greetham, Greg M. ^[1]; Middleton, Chris T. ^[2]; Luther, Bradley M. ^[3]; Zanni, Martin T.  ^[4];

• Search DOE PAGES for author "Zanni, Martin T."
• Search DOE PAGES for ORCID "0000-0001-7191-9768"

Hamm, Peter  ^[5];

• Search DOE PAGES for author "Hamm, Peter"
• Search DOE PAGES for ORCID "0000-0003-1106-6032"

Krummel, Amber T.  ^[3]

• Search DOE PAGES for author "Krummel, Amber T."
• Search DOE PAGES for ORCID "0000-0003-3973-1575"

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+ Show Author Affiliations

1. Central Laser Facility, Research Complex at Harwell, STFC Rutherford Appleton Laboratory, Harwell Science and Innovation Campus, Didcot OX11 0QX, United Kingdom
2. PhaseTech Spectroscopy, Inc., 4916 East Broadway, Suite 125, Madison, Wisconsin 53716, United States
3. Colorado State University, Department of Chemistry, 200 W. Lake Street, Fort Collins, Colorado 80523, United States
4. University of Wisconsin, Department of Chemistry, Room 8361, 1101 University Ave., Madison, Wisconsin 53706, United States
5. University of Zurich, Department of Chemistry, Winterthurerstrasse 190, Zurich CH-8057, Switzerland

Publication Date:

Mon Jul 10 00:00:00 EDT 2023

Research Org.:

Colorado State Univ., Fort Collins, CO (United States)

Sponsoring Org.:

USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:

2282655

Alternate Identifier(s):

OSTI ID: 2311846

Grant/Contract Number:  

SC0016137

Resource Type:

Published Article

Journal Name:

Accounts of Chemical Research

Additional Journal Information:

Journal Name: Accounts of Chemical Research Journal Volume: 56 Journal Issue: 15; Journal ID: ISSN 0001-4842

Publisher:

American Chemical Society

Country of Publication:

United States

Language:

English

Subject:

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Infrared light; Infrared spectroscopy; Lasers; Probes; Ultrafast spectroscopy