One of the most powerful tools to investigate the structural dynamics of electronically excited molecular systems is visible-pump/mid-infrared-probe spectroscopy. When performing this kind of experiments one must be aware of the artifacts deriving from the non-linear response of the solvent and of the sample cell itself. Cross-phase modulation (XPM) is observed when a strong visible-pump pulse modulates the refraction index seen by the mid-infrared-probe. The effect is enhanced when the probe pulse is chirped and causes the distortion of the transient signal in both the frequency and the time domains. We undertook a detailed simulation of XPM in the mid-infrared region where a visible pulse modulates the MIR pulse by XPM and in close conditions to the experimental ones. Our simulation takes into account the different group velocities of the pump and probe pulses and includes the influence of the linear chirp of the mid-infrared pulse and its asymmetry. The results of our numerical calculations fit very well the experimental signals measured in a 2 mm thick CaF2 window.

Cross-phase modulation in visible-pump/mid-infrared-probe spectroscopy / Lapini, Andrea; Mosquera Vázquez, Sandra; Tourón Touceda, Patricia; Lima, Manuela. - In: JOURNAL OF MOLECULAR STRUCTURE. - ISSN 0022-2860. - 993:1-3(2011), pp. 470-473. [10.1016/j.molstruc.2010.11.042]

Cross-phase modulation in visible-pump/mid-infrared-probe spectroscopy

Andrea Lapini;
2011

Abstract

One of the most powerful tools to investigate the structural dynamics of electronically excited molecular systems is visible-pump/mid-infrared-probe spectroscopy. When performing this kind of experiments one must be aware of the artifacts deriving from the non-linear response of the solvent and of the sample cell itself. Cross-phase modulation (XPM) is observed when a strong visible-pump pulse modulates the refraction index seen by the mid-infrared-probe. The effect is enhanced when the probe pulse is chirped and causes the distortion of the transient signal in both the frequency and the time domains. We undertook a detailed simulation of XPM in the mid-infrared region where a visible pulse modulates the MIR pulse by XPM and in close conditions to the experimental ones. Our simulation takes into account the different group velocities of the pump and probe pulses and includes the influence of the linear chirp of the mid-infrared pulse and its asymmetry. The results of our numerical calculations fit very well the experimental signals measured in a 2 mm thick CaF2 window.
File in questo prodotto:
File Dimensione Formato  
Journal of Molecular Structure 993 (2011) 470–473.pdf

solo utenti autorizzati

Tipologia: final published article (publisher’s version)
Licenza: Non Pubblico - Accesso privato/ristretto
Dimensione 351.89 kB
Formato Adobe PDF
351.89 kB Adobe PDF   Visualizza/Apri   Richiedi una copia

I documenti in IRIS sono protetti da copyright e tutti i diritti sono riservati, salvo diversa indicazione.

Utilizza questo identificativo per citare o creare un link a questo documento: https://hdl.handle.net/11696/58655
Citazioni
  • ???jsp.display-item.citation.pmc??? ND
  • Scopus 10
  • ???jsp.display-item.citation.isi??? 10
social impact