Separating Orders of Response in Transient Absorption and Coherent Multidimensional Spectroscopy by Intensity Variation

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F00216208%3A11320%2F25%3A10509830" target="_blank" >RIV/00216208:11320/25:10509830 - isvavai.cz</a>

Výsledek na webu

<a href="https://verso.is.cuni.cz/pub/verso.fpl?fname=obd_publikace_handle&handle=hZnfinlEt7" target="_blank" >https://verso.is.cuni.cz/pub/verso.fpl?fname=obd_publikace_handle&handle=hZnfinlEt7</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1021/acs.jpclett.5c01177" target="_blank" >10.1021/acs.jpclett.5c01177</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Separating Orders of Response in Transient Absorption and Coherent Multidimensional Spectroscopy by Intensity Variation

Popis výsledku v původním jazyce

Interpretation of time-resolved spectroscopies such as transient absorption (TA) or two-dimensional (2D) spectroscopy often relies on the perturbative description of light-matter interaction. In many cases the third order of nonlinear response is the leading and desired term. When pulse amplitudes are high, higher orders of light-matter interaction can both distort lineshapes and dynamics and provide valuable information. Here, we present a general procedure to separately measure the nonlinear response orders in both TA and 2D spectroscopies, using linear combinations of intensity-dependent spectra. We analyze the residual contamination and random errors and show how to choose optimal intensities to minimize the total error in the extracted orders. For an experimental demonstration, we separate the nonlinear orders in the 2D electronic spectroscopy of squaraine polymers up to the 11th order.

Název v anglickém jazyce

Separating Orders of Response in Transient Absorption and Coherent Multidimensional Spectroscopy by Intensity Variation

Popis výsledku anglicky

Interpretation of time-resolved spectroscopies such as transient absorption (TA) or two-dimensional (2D) spectroscopy often relies on the perturbative description of light-matter interaction. In many cases the third order of nonlinear response is the leading and desired term. When pulse amplitudes are high, higher orders of light-matter interaction can both distort lineshapes and dynamics and provide valuable information. Here, we present a general procedure to separately measure the nonlinear response orders in both TA and 2D spectroscopies, using linear combinations of intensity-dependent spectra. We analyze the residual contamination and random errors and show how to choose optimal intensities to minimize the total error in the extracted orders. For an experimental demonstration, we separate the nonlinear orders in the 2D electronic spectroscopy of squaraine polymers up to the 11th order.

Druh

J_imp - Článek v periodiku v databázi Web of Science

CEP obor

—

OECD FORD obor

10301 - Atomic, molecular and chemical physics (physics of atoms and molecules including collision, interaction with radiation, magnetic resonances, Mössbauer effect)

Projekt

—

Návaznosti

I - Institucionalni podpora na dlouhodoby koncepcni rozvoj vyzkumne organizace

Rok uplatnění

2025

Kód důvěrnosti údajů

S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů

Název periodika

Journal of Physical Chemistry Letters

ISSN

1948-7185

e-ISSN

—

Svazek periodika

16

Číslo periodika v rámci svazku

24

Stát vydavatele periodika

US - Spojené státy americké

Počet stran výsledku

9

Strana od-do

5897-5905

Kód UT WoS článku

001508305600001

EID výsledku v databázi Scopus

2-s2.0-105007515214