Local coherence and the temporal development of second harmonic emission

被引:7
作者
Andrews, DL [1 ]
Romero, LD [1 ]
机构
[1] Univ E Anglia, Sch Chem Sci, Norwich NR4 7TJ, Norfolk, England
关键词
D O I
10.1088/0953-4075/34/11/310
中图分类号
O43 [光学];
学科分类号
070207 ; 0803 ;
摘要
In a variety of mesoscopically disordered systems, high levels of optical excitation resulting from pulsed laser irradiation can establish optical coherence within separate particles or locally ordered domains, leading to second harmonic emission whose temporal signature characterizes the decay of the excited state population. Examples of such systems will include colloids, cell and membrane suspensions, and many plastics, glasses and other modern materials. With pulsed excitation of sufficient intensity to elicit the onset of saturation, second harmonic emission on the throughput of;a subsequent probe beam exhibits a characteristic decay and recovery. Detailed calculations show that such features arise not only in systems whose optical response involves two discrete levels, but also in systems of considerably greater electronic complexity. Deconvolution of the temporal trace of the harmonic signal serves as an independent means of monitoring the decay of the excited state. The extent of recovery in the harmonic signal also serves to register the extent of local coherence, and hence in many systems the localization of structural order. Finally, the principles introduced in the theory are shown to be applicable to other types of system such as certain photochromic materials.
引用
收藏
页码:2177 / 2187
页数:11
相关论文
共 37 条
[1]   Doubly forbidden second-harmonic generation from isotropic suspensions: Studies on the purple membrane of Halobacterium halobium [J].
Allcock, P ;
Andrews, DL ;
Meech, SR ;
Wigman, AJ .
PHYSICAL REVIEW A, 1996, 53 (04) :2788-2791
[2]   Six-wave mixing: secular resonances in a higher-order mechanism for second-harmonic generation [J].
Allcock, P ;
Andrews, DL .
JOURNAL OF PHYSICS B-ATOMIC MOLECULAR AND OPTICAL PHYSICS, 1997, 30 (16) :3731-3742
[3]  
Andrews D. L., 1994, Nonlinear Optics, Principles, Materials, Phenomena and Devices, V8, P25
[4]   THE ROLE OF LONGITUDINAL POLARIZATION IN SURFACE 2ND-HARMONIC GENERATION [J].
ANDREWS, DL .
JOURNAL OF MODERN OPTICS, 1993, 40 (05) :939-946
[5]   THEORY OF 2ND-HARMONIC GENERATION IN RANDOMLY ORIENTED SPECIES [J].
ANDREWS, DL ;
ALLCOCK, P ;
DEMIDOV, AA .
CHEMICAL PHYSICS, 1995, 190 (01) :1-9
[6]   ON THE ROLE OF PERMANENT DIPOLES IN 2ND-HARMONIC GENERATION [J].
ANDREWS, DL ;
MEATH, WJ .
JOURNAL OF PHYSICS B-ATOMIC MOLECULAR AND OPTICAL PHYSICS, 1993, 26 (23) :4633-4641
[7]   An algorithm for the nonlinear optical susceptibilities of dipolar molecules, and an application to third harmonic generation [J].
Andrews, DL ;
Romero, LCD ;
Meath, WJ .
JOURNAL OF PHYSICS B-ATOMIC MOLECULAR AND OPTICAL PHYSICS, 1999, 32 (01) :1-17
[8]  
[Anonymous], ADV CHEM PHYS
[9]   COUPLING BETWEEN PHOTOCHROMISM AND 2ND-HARMONIC GENERATION IN SPIROPYRAN-DOPED AND SPIROOXAZINE-DOPED POLYMER-FILMS [J].
ATASSI, Y ;
DELAIRE, JA ;
NAKATANI, K .
JOURNAL OF PHYSICAL CHEMISTRY, 1995, 99 (44) :16320-16326
[10]   Spiropyrans and spirooxazines for memories and switches [J].
Berkovic, G ;
Krongauz, V ;
Weiss, V .
CHEMICAL REVIEWS, 2000, 100 (05) :1741-1753