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

Journal Article · · Accounts of Chemical Research
ORCiD logo [1];  [1];  [2];  [3]; ORCiD logo [4]; ORCiD logo [5]; ORCiD logo [3]
  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

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 describe 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.

Research Organization:
Colorado State Univ., Fort Collins, CO (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
SC0016137
OSTI ID:
2282655
Alternate ID(s):
OSTI ID: 2311846
Journal Information:
Accounts of Chemical Research, Journal Name: Accounts of Chemical Research Vol. 56 Journal Issue: 15; ISSN 0001-4842
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English

References (71)

Sub-10-fs pulses tunable from 480 to 980  nm from a NOPA pumped by an Yb:KGW source journal July 2014
Coherent two-dimensional electronic mass spectrometry journal June 2018
Direct Observation of Reactive Intermediates by Time-Resolved Spectroscopy Unravels the Mechanism of a Radical-Induced 1,2-Metalate Rearrangement journal October 2021
Photon echoes and two dimensional spectra of the amide I band of proteins measured by femtosecond IR – Raman spectroscopy journal January 2020
High-Throughput Two-Dimensional Infrared (2D IR) Spectroscopy Achieved by Interfacing Microfluidic Technology with a High Repetition Rate 2D IR Spectrometer journal November 2016
Enabling high repetition rate nonlinear THz science with a kilowatt-class sub-100 fs laser source journal May 2020
Two-color two-dimensional Fourier transform electronic spectroscopy with a pulse-shaper journal January 2008
Theory and phase-cycling scheme selection principles of collinear phase coherent multi-dimensional optical spectroscopy journal September 2008
Analysis of amyloid-like secondary structure in the Cryab-R120G knock-in mouse model of hereditary cataracts by two-dimensional infrared spectroscopy journal September 2021
Picosecond to millisecond tracking of a photocatalytic decarboxylation reaction provides direct mechanistic insights journal November 2019
Long-Range Vibrational Dynamics Are Directed by Watson–Crick Base Pairing in Duplex DNA journal April 2016
Coherent two-dimensional photocurrent spectroscopy in a PbS quantum dot photocell journal December 2014
Broadband near-field infrared spectromicroscopy using photothermal probes and synchrotron radiation journal January 2016
Direct Observation of the Microscopic Reverse of the Ubiquitous Concerted Metalation Deprotonation Step in C–H Bond Activation Catalysis journal January 2021
500 kHz OPCPA delivering tunable sub-20 fs pulses with 15 W average power based on an all-ytterbium laser journal January 2015
Transient 2D IR spectroscopy from micro- to milliseconds journal March 2021
A 100 kHz Pulse Shaping 2D-IR Spectrometer Based on Dual Yb:KGW Amplifiers journal January 2018
Watching Proteins Wiggle: Mapping Structures with Two-Dimensional Infrared Spectroscopy journal January 2017
Time-Domain Vibrational Action Spectroscopy of Cryogenically Cooled, Messenger-Tagged Ions Using Ultrafast IR Pulses journal November 2021
Water vibrations have strongly mixed intra- and intermolecular character journal September 2013
Ytterbium solid-state lasers. The first decade journal November 2000
Subpicosecond kilowatt pulses from a mode-locked cw dye laser journal April 1974
Adding a dimension to the infrared spectra of interfaces using heterodyne detected 2D sum-frequency generation (HD 2D SFG) spectroscopy journal December 2011
Impact of non-equilibrium molecular packings on singlet fission in microcrystals observed using 2D white-light microscopy journal December 2019
100-kHz shot-to-shot broadband data acquisition for high-repetition-rate pump–probe spectroscopy journal January 2014
Residue-specific structural kinetics of proteins through the union of isotope labeling, mid-IR pulse shaping, and coherent 2D IR spectroscopy journal September 2010
Infrared spectroscopy reveals multi-step multi-timescale photoactivation in the photoconvertible protein archetype dronpa journal June 2018
Mechanism of IAPP amyloid fibril formation involves an intermediate with a transient  -sheet journal November 2013
4-W, 100-kHz, few-cycle mid-infrared source with sub-100-mrad carrier-envelope phase noise journal January 2017
Thermal Annealing of Singlet Fission Microcrystals Reveals the Benefits of Charge Transfer Couplings and Slip-Stacked Packing journal June 2020
2D IR spectroscopy at 100 kHz utilizing a Mid-IR OPCPA laser source journal January 2016
Concepts and Methods of 2D Infrared Spectroscopy book January 2011
Purely absorptive three-dimensional infrared spectroscopy journal April 2009
Spatially Resolved Two-Dimensional Infrared Spectroscopy via Wide-Field Microscopy journal June 2016
High-energy few-cycle pulses: post-compression techniques journal November 2020
Fluorescence-detected two-dimensional electronic coherence spectroscopy by acousto-optic phase modulation journal December 2007
A 100 kHz Time-Resolved Multiple-Probe Femtosecond to Second Infrared Absorption Spectrometer journal February 2016
Shot-to-shot 2D IR spectroscopy at 100 kHz using a Yb laser and custom-designed electronics journal October 2020
Sequence of Events during Peptide Unbinding from RNase S: A Complete Experimental Description journal May 2021
Dual spectral phase and diffraction angle compensation of a broadband AOM 4-f pulse-shaper for ultrafast spectroscopy journal December 2019
Broadband 2D electronic spectrometer using white light and pulse shaping: noise and signal evaluation at 1 and 100 kHz journal January 2017
Long seed, short pump: converting Yb-doped laser radiation to multi-µJ few-cycle pulses tunable through 2.5–15 µm journal April 2022
Time-resolved infra-red studies of photo-excited porphyrins in the presence of nucleic acids and in HeLa tumour cells: insights into binding site and electron transfer dynamics journal January 2022
Noise analysis and noise reduction methods in kilohertz pump-probe experiments journal July 2007
Three-dimensional electronic spectroscopy of excitons in GaAs quantum wells journal October 2009
Manganese-Mediated C–H Bond Activation of Fluorinated Aromatics and the ortho-Fluorine Effect: Kinetic Analysis by In Situ Infrared Spectroscopic Analysis and Time-Resolved Methods journal January 2022
Application of 2D IR Bioimaging: Hyperspectral Images of Formalin-Fixed Pancreatic Tissues and Observation of Slow Protein Degradation journal August 2021
60-fsec pulse generation from a self-mode-locked Ti:sapphire laser journal January 1991
Femtosecond to microsecond observation of the photochemical reaction of 1,2-di(quinolin-2-yl)disulfide with methyl methacrylate journal January 2017
Single-stage MHz mid-IR OPA using LiGaS2and a fiber laser pump source journal March 2018
Rapid-scan coherent 2D fluorescence spectroscopy journal January 2017
Compression of optical pulses to six femtoseconds by using cubic phase compensation journal January 1987
Supercontinuum-seeded few-cycle mid-infrared OPCPA system journal January 2016
Transient 2D-IR Spectroscopy:  Snapshots of the Nonequilibrium Ensemble during the Picosecond Conformational Transition of a Small Peptide journal August 2003
How to turn your pump–probe instrument into a multidimensional spectrometer: 2D IR and Vis spectroscopiesvia pulse shaping journal January 2009
Short-Range Catalyst–Surface Interactions Revealed by Heterodyne Two-Dimensional Sum Frequency Generation Spectroscopy journal October 2015
Ultrafast vibrational dynamics of water at a charged interface revealed by two-dimensional heterodyne-detected vibrational sum frequency generation journal September 2012
Ultrafast 2D IR microscopy journal January 2014
Pentacarbonylchromium-solvent complexes journal April 1974
Heterodyned 3D IR spectroscopy journal November 2007
Purely absorptive fifth-order three-dimensional electronic spectroscopy journal December 2012
Femtochemistry:  Atomic-Scale Dynamics of the Chemical Bond journal June 2000
A stop-flow sample delivery system for transient spectroscopy journal December 2021
The molecular mechanism of light-induced bond formation and breakage in the cyanobacteriochrome TePixJ journal January 2023
Multidimensional Spectroscopy on the Microscale: Development of a Multimodal Imaging System Incorporating 2D White-Light Spectroscopy, Broadband Transient Absorption, and Atomic Force Microscopy journal November 2019
Transient 2D IR spectroscopy and multiscale simulations reveal vibrational couplings in the Cyanobacteriochrome Slr1393-g3 preprint January 2023
Compression of amplified chirped optical pulses journal October 1985
Amplification of mid-IR continuum for broadband 2D IR spectroscopy journal February 2023
Multidimensional Electronic Spectroscopy of Photochemical Reactions journal August 2015
2D Electronic Spectroscopic Techniques for Quantum Technology Applications journal June 2021
Observation of optical coherence in a disordered metal-molecule interface by coherent optical two-dimensional photoelectron spectroscopy journal May 2022